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Abstract Electronic devices are ubiquitous in modern society, yet their poor recycling rates contribute to substantial economic losses and worsening environmental impacts from electronic waste (E‐waste) disposal. Here, recyclable and healable electronics are reported through a vitrimer‐liquid metal (LM) microdroplet composite. These electrically conductive, yet plastic‐like composites display mechanical qualities of rigid thermosets and recyclability through a dynamic covalent polymer network. The composite exhibits a high glass transition temperature, good solvent resistance, high electrical conductivity, and recyclability. The vitrimer synthesis proceeds without the need for a catalyst or a high curing temperature, which enables facile fabrication of the composite materials. The as‐synthesized vitrimer exhibits a fast relaxation time with reconfigurability and shape memory. The electrically conductive composite exhibits high electrical conductivity with LM volume loading as low as 5 vol.%. This enables the fabrication of fully vitrimer‐based circuit boards consisting of sensors and indicator LEDs integrated with LM‐vitrimer conductive wiring. Electrical self‐healing and thermally triggered material healing are further demonstrated with the composites. The vitrimer and LM‐composite provide a pathway toward fully recyclable, mechanically robust, and reconfigurable electronics, thus advancing the field of electronic materials. 

Abstract Linear poly(α‐hydroxy acids) are important degradable polymers, and they can be efficiently prepared by ring‐opening polymerization of O‐carboxyanhydrides with pendant functional groups. However, attempts to prepare cyclic poly(α‐hydroxy acids) have been plagued by side reactions, including epimerization and uncontrolled intramolecular chain transfers or termination, that prevent the synthesis of high‐molecular‐weight stereoregular cyclic polyesters. Herein, we report a scalable method for the synthesis of high‐molecular‐weight (>100 kDa) stereoregular functionalized cyclic poly(α‐hydroxy acids) by means of controlled polymerization of O‐carboxyanhydrides using a catalytic system consisting of a lanthanum complex with a sterically bulky ligand and a manganese silylamide. Additionally, using this system, we could readily prepare cyclic block poly(α‐hydroxy acids) by means of sequential addition of O‐carboxyanhydrides. The obtained cyclic polyesters and their cyclic block copolyesters exhibit distinctive physicochemical properties—including elevated phase transition temperature, improved toughness, and reduced viscosity—compared to their linear counterparts.