Di Wen, Xiaotong Yu, Hao He, Yuan Gao, Kun Cao, Rong Chen
ABSTRACT Achieving stable light emission under large, repeated, and multiaxial deformation remains challenging due to the intrinsic brittleness and environmental sensitivity of emissive materials. Here, we report a region‐selective fabrication strategy that integrates block copolymer (BCP)‐guided emissive‐domain formation with selective atomic layer infiltration (ALI). This strategy enables the construction of stretchable rigid‐soft luminescent films with mechanically compliant matrices and locally protected emissive domains. Block‐copolymer self‐assembly defines spatially isolated emissive domains, while ALI selectively forms nanoscopic oxide armors only within emitter‐containing regions, reinforcing the domains without stiffening the surrounding soft matrix. Finite‐element analysis and strain‐dependent optical measurements indicate that applied strain is predominantly accommodated by the soft matrix, leaving the rigid emitter domains effectively unstrained. The resulting stretchable luminescent films maintain nearly unchanged optical performance under up to 100% multiaxial strain. The region‐selective construction strategy provides a general design route for mechanically robust luminescent systems.