A state-of-the-art review of multi-cross-linked hydrophobic associated hydrogels for soft electronic, biomedical, and environmental applications.

Thanks to their considerable toughness, self-recoverability, high swelling degree and stimuli-responsiveness, hydrophobic association (HA) hydrogels are promising in wearable electronics, biomedical applications and the water treatment industry. Multiple (physical and/or chemical) cross-links can also promote the above-mentioned properties, broadening the applications of the gels. Previous reviews on the HA hydrogels focused only on their mechanical and self-healing properties for biomedical applications. Herein, we aim to introduce HA hydrogels having multiple crosslinks (multi-cross-linked HA (MCHA) gels), discuss their various properties, and then present their (potential) practical applications. To explain, this review first describes the synthesis of MCHA gels. Then, the mechanical, rheological, self-healing, injectability, swelling, and stimuli-responsive properties of MCHA hydrogels are discussed. In the meantime, we suggest useful approaches to address the current challenges for the sake of improving these properties. Finally, based on the properties of MCHA gels, we introduce their (potential) applications in the fields of soft electronics, biomedicine, the environment, and superabsorbents, followed by evaluation of the performance of the developed devices in some cases. Taken together, this review can provide helpful perspectives for developing high-performance MCHA hydrogels.

• Publication year

  2025

• Venue

  Journal of materials chemistry. B

• Publication date

  2025-07-14

• Fields of study

  Medicine, Materials Science, Engineering, Environmental Science

• Identifiers
  DOI 10.1039/d5tb00506jPMID 40654160
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar, PubMed

• No claims are published for this paper.

• No concepts are published for this paper.

• Temperature-triggered inflatable hydrogel muscles with snap-through instability for untethered robots

  2025cited by this paper
• Surfactant-rescued gelation: Stabilizing P123-chitosan hydrogels in blood-isotonic aqueous solutions for controlled drug delivery.

  2025cited by this paper
• Micelle-Containing Hydrogels and Their Applications in Biomedical Research

  2024cited by this paper
• Dually-crosslinked ionic conductive hydrogels reinforced through biopolymer gellan gum for flexible sensors to monitor human activities.

  2024cited by this paper
• Hydrophobic association-improved multi-functional hydrogels with liquid metal droplets stabilized by xanthan gum and PEDOT:PSS for strain sensors.

  2024cited by this paper
• Liquid Metal Nanoparticles Physically Hybridized with Cellulose Nanocrystals Initiate and Toughen Hydrogels with Piezoionic Properties.

  2024cited by this paper
• Development of a Nano-toughened multifunctional composite hydrogel based on chitosan and its applications in catalytic and flexible sensors.

  2024cited by this paper
• Starch/ionic liquid/hydrophobic association hydrogel with high stretchability, fatigue resistance, self-recovery and conductivity for sensitive wireless wearable sensors.

  2024cited by this paper
• Triple physical cross-linking cellulose nanofibers-based poly(ionic liquid) hydrogel as wearable multifunctional sensors.

  2024cited by this paper
• Notch-insensitive, tough and self-healing conductive bacterial cellulose nanocomposite hydrogel for flexible wearable strain sensor.

  2024cited by this paper
• Tough, Healable, and Sensitive Strain Sensor Based on Multiphysically Cross-Linked Hydrogel for Ionic Skin.

  2023cited by this paper
• Novel Uracil-Functionalized Poly(ionic liquid) Hydrogel: Highly Stretchable and Sensitive as a Direct Wearable Ionic Skin for Human Motion Detection.

  2023cited by this paper
• Harnessing the Interplay of Triple Cross-Linked Hydrogels toward Multiresponsive Alginate-Based Injectable Gels for 3D Printing Bioapplications.

  2023cited by this paper
• Multi-Physically Cross-Linked Hydrogels for Flexible Sensors with High Strength and Self-Healing Properties

  2023cited by this paper
• Tailoring the Swelling‐Shrinkable Behavior of Hydrogels for Biomedical Applications

  2023cited by this paper
• Polymer-Based Hydrogels Applied in Drug Delivery: An Overview

  2023cited by this paper
• An Anti‐Fracture and Super Deformable Soft Hydrogel Network Insensitive to Extremely Harsh Environments

  2023cited by this paper
• Extraction, Modification and Biomedical Application of Agarose Hydrogels: A Review

  2023cited by this paper
• Conductive polymer based hydrogels and their application in wearable sensors: a review.

  2023cited by this paper
• Hydrophobically Associated Hydrogel for High Sensitivity and Resolution of an Interdigital Electrode Pressure Sensor.

  2023cited by this paper
• Preparation and properties of a photocrosslinked MCln-doped PDMA-g-PSMA hydrogel

  2023cited by this paper
• 4D Printing of Body Temperature-Responsive Hydrogels Based on Poly(acrylic acid) with Shape-Memory and Self-Healing Abilities

  2023cited by this paper
• A rapidly and Highly Self-Healing Poly(Sulfobetaine Methacrylate) Hydrogel with Stretching Properties, Adhesive Properties and Biocompatibility.

  2022cited by this paper
• Tough and self-healing hydrogels based on transient crosslinking by nanoparticles.

  2022cited by this paper
• Superstrong, superstiff, and conductive alginate hydrogels

  2022cited by this paper
• Tough, Anti-Swelling Supramolecular Hydrogels Mediated by Surfactant-Polymer Interactions for Underwater Sensors.

  2022cited by this paper
• Mussel-Inspired Adhesive and Self-Healing Hydrogel as an Injectable Wound Dressing

  2022cited by this paper
• Unbreakable Hydrogels with Self‐Recoverable 10 200% Stretchability

  2022cited by this paper
• Regulable Supporting Baths for Embedded Printing of Soft Biomaterials with Variable Stiffness.

  2022cited by this paper
• Tunable Physicomechanical and Drug Release Properties of In Situ Forming Thermoresponsive Elastin-like Polypeptide Hydrogels.

  2022cited by this paper
• A Universal and Simple Method to Obtain Hydrogels with Combined Extreme Mechanical Properties and Their Application as Tendon Substitutes.

  2022cited by this paper
• Cellulose nanocrystals boosted hydrophobic association in dual network polymer hydrogels as advanced flexible strain sensor for human motion detection.

  2022cited by this paper
• pH-Responsive, Thermo-Resistant Poly(Acrylic Acid)-g-Poly(boc-L-Lysine) Hydrogel with Shear-Induced Injectability

  2022cited by this paper
• A review on the features, performance and potential applications of hydrogel-based wearable strain/pressure sensors.

  2021cited by this paper
• High-Strength Hydrogel Adhesive Formed via Multiple Interactions for Persistent Adhesion under Saline.

  2021cited by this paper
• Hydrophobically-Modified PEG Hydrogels with Controllable Hydrophilic/Hydrophobic Balance

  2021cited by this paper
• A highly sensitive strain sensor based on a silica@polyaniline core-shell particle reinforced hydrogel with excellent flexibility, stretchability, toughness and conductivity.

  2021cited by this paper
• Relationship between Structure and Rheology of Hydrogels for Various Applications

  2021cited by this paper
• Current hydrogel advances in physicochemical and biological response-driven biomedical application diversity

  2021cited by this paper
• Polydopamine/polystyrene nanocomposite double-layer strain sensor hydrogel with mechanical, self-healing, adhesive and conductive properties.

  2020cited by this paper
• Fully physically crosslinked pectin-based hydrogel with high stretchability and toughness for biomedical application.

  2020cited by this paper
• Fully physically cross-linked double network hydrogels with strong mechanical properties, good recovery and self-healing properties.

  2020cited by this paper
• Bio-inspired adhesive and self-healing hydrogels as flexible strain sensors for monitoring human activities.

  2020cited by this paper
• Fundamental Concepts of Hydrogels: Synthesis, Properties, and Their Applications

  2020cited by this paper
• Highly Sensitive Pressure and Strain Sensors Based on Stretchable and Recoverable Ion-Conductive Physically Cross-Linked Double-Network Hydrogels.

  2020cited by this paper
• A Review of Conductive Hydrogel Used in Flexible Strain Sensor

  2020cited by this paper
• Reinforced macromolecular micelle-crosslinked hyaluronate gels induced by water/DMSO binary solvent.

  2020cited by this paper
• Robust and anti-fatigue hydrophobic association hydrogels assisted by titanium dioxide for photocatalytic activity.

  2019cited by this paper
• Autonomic Self-Healing Silk Fibroin Injectable Hydrogels Formed via Surfactant-Free Hydrophobic Association.

  2019cited by this paper
• Tough hydrophobic association hydrogels with self-healing and reforming capabilities achieved by polymeric core-shell nanoparticles.

  2019cited by this paper
• Highly tough, anti-fatigue and rapidly self-recoverable hydrogels reinforced with core-shell inorganic-organic hybrid latex particles.

  2017cited by this paper
• Super-tough, ultra-stretchable and strongly compressive hydrogels with core-shell latex particles inducing efficient aggregation of hydrophobic chains.

  2017cited by this paper

• Intelligent Self-Healing Hydrogels: AI-Empowered Design, Biomedical Innovation, and Future Horizons

  2026cites this paper
• Purpose-Driven Design and Manufacturing of Hydrogel Sorbents for Efficient Atmospheric Water Harvesting.

  2025cites this paper
• Self-Healing Polymer-Based Coatings: Mechanisms and Applications Across Protective and Biofunctional Interfaces

  2025cites this paper