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Self-healing soft electronic and robotic devices can, like human skin, recover autonomously from damage. While current devices use a single type of dynamic polymer for all functional layers to ensure strong interlayer adhesion, this approach requires manual layer alignment. In this study, we used two dynamic polymers, which have immiscible backbones but identical dynamic bonds, to maintain interlayer adhesion while enabling autonomous realignment during healing. These dynamic polymers exhibit a weakly interpenetrating and adhesive interface, whose width is tunable. When multilayered polymer films are misaligned after damage, these structures autonomously realign during healing to minimize interfacial free energy. We fabricated devices with conductive, dielectric, and magnetic particles that functionally heal after damage, enabling thin-film pressure sensors, magnetically assembled soft robots, and underwater circuit assembly.

The practical implementation of Li metal batteries is hindered by difficulties in controlling the Li metal plating microstructure. While previous atomic layer deposition (ALD) studies have focused on directly coating Li metal with thin films for the passivation of the electrode–electrolyte interface, a different approach is adopted, situating the ALD film beneath Li metal and directly on the copper current collector. A mechanistic explanation for this simple strategy of controlling the Li metal plating microstructure using TiO₂grown on copper foil by ALD is presented. In contrast to previous studies where ALD‐grown layers act as artificial interphases, this TiO₂layer resides at the copper–Li metal interface, acting as a nucleation layer to improve the Li metal plating morphology. Upon lithiation of TiO₂, a Li_xTiO₂complex forms; this alloy provides a lithiophilic surface layer that enables uniform and reversible Li plating. The reversibility of lithium deposition is evident from the champion cell (5 nm TiO₂), which displays an average Coulombic efficiency (CE) of 96% after 150 cycles at a moderate current density of 1 mA cm⁻². This simple approach provides the first account of the mechanism of ALD‐derived Li nucleation control and suggests new possibilities for future ALD‐synthesized nucleation layers.

The solid electrolyte interphase (SEI) has been identified as a key challenge for Li metal anodes. The brittle and inhomogeneous native SEI generated by parasitic reactions between Li and liquid electrolytes can devastate battery performance; therefore, artificial SEIs (ASEIs) have been proposed as an effective strategy to replace native SEIs. Herein, as a collaboration between academia and industrial R&D teams, a multifunctional (crystalline, high modulus, and robust, Li⁺ion conductive, electrolyte‐blocking, and solution processable) ASEI material, LiAl‐FBD (where “FBD” refers to 2,2,3,3‐tetrafluoro‐1,4‐butanediol), for improving Li metal battery performance is designed and synthesized. The LiAl‐FBD crystal structure consists of Al³⁺ions bridged by FBD^2–ligands to form anion clusters while Li⁺ions are loosely bound at the periphery, enabling an Li⁺ion conductivity of 9.4 × 10^–6S cm^–1. The fluorinated, short ligands endow LiAl‐FBD with electrolyte phobicity and high modulus. The ASEI is found to prevent side reactions and extend the cycle life of Li metal electrodes. Specifically, pairing LiAl‐FBD coated 50 µm thick Li with industrial 3.5 mAh cm^–2NMC811 cathode and 2.8 µL mAh^–1lean electrolyte, the Li metal full cells show superior cycle life compared to bare ones, achieving 250 cycles at 1 mA cm^–2.