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Abstract The innate immune system plays a dual role in both mediating pathogenic processes following tissue damage and acting as a barrier to effective therapeutic delivery. Strategies that evade immune clearance while modulating host immune components offer promising solutions for treating complex chronic diseases, such as fibrosis. Here, an innate immune checkpoint material‐based strategy is presented in which mesenchymal stromal cells, coated with a soft conformal microgel and functionalized with the CD47 self‐marker agonist, effectively evade clearance by tissue resident macrophages. These engineered cells reverse persistent fibrotic damage in the lungs through a paracrine mechanism. Single‐cell RNA sequencing identifies a transitional antigen‐presenting macrophage subpopulation that mediates these reparative effects. By combining immune cloaking with the presentation of local signals encoded in the gel coatings, this strategy can be used to design secretory cells for long‐term tissue remodeling, enabling a living pharmacy for chronic tissue damage. 

Abstract This study presents a novel polymer‐in‐salt (PIS) zwitterionic polyurethane‐based solid polymer electrolyte (zPU‐SPE) that offers high ionic conductivity, strong interaction with electrodes, and excellent mechanical and electrochemical stabilities, making it promising for high‐performance all solid‐state lithium batteries (ASSLBs). The zPU‐SPE exhibits remarkable lithium‐ion (Li⁺) conductivity (3.7 × 10⁻⁴ S cm⁻¹at 25 °C), enabled by exceptionally high salt loading of up to 90 wt.% (12.6 molar ratio of Li salt to polymer unit) without phase separation. It addresses the limitations of conventional SPEs by combining high ionic conductivity with a Li⁺transference number of 0.44, achieved through the incorporation of zwitterionic groups that enhance ion dissociation and transport. The high surface energy (338.4 J m⁻²) and elasticity ensure excellent adhesion to Li anodes, reducing interfacial resistance and ensuring uniform Li⁺flux. When tested in Li||zPU||LiFePO₄ and Li||zPU||S/C cells, the zPU‐SPE demonstrated remarkable cycling stability, retaining 76% capacity after 2000 cycles with the LiFePO₄cathode, and achieving 84% capacity retention after 300 cycles with the S/C cathode. Molecular simulations and a range of experimental characterizations confirm the superior structural organization of the zPU matrix, contributing to its outstanding electrochemical performance. The findings strongly suggest that zPU‐SPE is a promising candidate for next‐generation ASSLBs.