A Sustainable Adhesive Paradigm: Reversibly Reinforcing, Heat‐Free Bonding with Universal Substrates

Abstract Non‐biodegradable adhesives accumulate in ecosystems and contribute to contamination. They even contaminate recyclable materials, reducing the efficiency of recycling processes or rendering them impossible. Transitioning to biodegradable or recyclable adhesives is critical to mitigating these environmental impacts and advancing zero‐waste initiatives. A nacre‐inspired hard‐soft multiphase structure is developed to serve as a heat‐free adhesive system, delivering superior adhesion strength across metal, plastic, and glass substrates. Autonomous reconstruction of physically cross‐linked networks and strain‐induced orientation synergistically achieve up to 120 de‐bonding and re‐bonding cycles with progressive adhesion enhancement. Repeatable bonding with reinforcement instead of strength reduction enables error‐tolerant applications. Unique thermal responsiveness that maintains exceptional adhesion performance under low‐temperature conditions, especially in liquid nitrogen environments, is investigated. The dynamic equilibrium of non‐covalent interactions coupled with hydrolytically sensitive ester bonds permits tunable degradation kinetics through compositional modulation. This design paradigm establishes an eco‐friendly alternative to conventional adhesives, particularly suitable for applications demanding recyclability, environmental compatibility, repeated usability, and operation under ultra‐low temperature conditions.