Rewriting Polymer Fate via Chemomechanical Coupling

Abstract

ABSTRACT How can synthetic polymers be endowed with the continuous, life‐like ability to grow, degrow, heal, and alter their chemical and physical properties after fabrication? This study addresses this question by coupling theory and experiment to create an open‐system “living” polymer platform that integrates mass transport, reversible polymerization, chain exchange, and evolving elasticity into a fully chemomechanically coupled network. Controlled transport, reaction, and stresses enable continuous growth and degrowth with microscale control enabled by light‐activated catalysts. Their chemical composition can be reprogrammed on demand, tuning modulus by up to two orders of magnitude to either stiffen or soften the material. These capabilities enable self‐growable electronics, transformative soft robots, and on‐site damage‐regenerating devices, establishing a foundation for sustainable, endlessly reprogrammable polymers.