Through advances in molecular design, understanding of processing parameters, and development of non‐traditional device fabrication techniques, the field of wearable and implantable skin‐inspired devices is rapidly growing interest in the consumer market. Like previous technological advances, economic growth and efficiency is anticipated, as these devices will enable an augmented level of interaction between humans and the environment. However, the parallel growing electronic waste that is yet to be addressed has already left an adverse impact on the environment and human health. Looking forward, it is imperative to develop both human‐ and environmentally‐friendly electronics, which are contingent on emerging recyclable, biodegradable, and biocompatible polymer technologies. This review provides definitions for recyclable, biodegradable, and biocompatible polymers based on reported literature, an overview of the analytical techniques used to characterize mechanical and chemical property changes, and standard policies for real‐life applications. Then, various strategies in designing the next‐generation of polymers to be recyclable, biodegradable, or biocompatible with enhanced functionalities relative to traditional or commercial polymers are discussed. Finally, electronics that exhibit an element of recyclability, biodegradability, or biocompatibility with new molecular design are highlighted with the anticipation of integrating emerging polymer chemistries into future electronic devices.

Mechanochemistry offers exciting opportunities for molecular-level engineering of stress-responsive properties of polymers. Reactive sites, sometimes called mechanophores, have been reported to increase the material toughness, to make the material mechanochromic or optically healable. Here we show that macrocyclic cinnamate dimers combine these productive stress-responsive modes. The highly thermally stable dimers dissociate on the sub-second timescale when subject to a stretching force of 1–2 nN (depending on isomer). Stretching a polymer of the dimers above this force more than doubles its contour length and increases the strain energy that the chain absorbs before fragmenting by at least 600 kcal per mole of monomer. The dissociation produces a chromophore and dimers are reformed upon irradiation, thus allowing optical healing of mechanically degraded parts of the material. The mechanochemical kinetics, single-chain extensibility, toughness and potentially optical properties of the dissociation products are tunable by synthetic modifications.