Thermoresponsive Liquid Crystalline Polymer Coatings Programmed by Field‐Induced Topological Defects for Tunable Optical and Topographical Responses

Self‐assembly of nano‐ and microstructures in soft materials enables stimuli‐responsive functionalities, yet scalable bottom‐up approaches that combine high spatial precision with robust solid‐state architectures remain limited. Liquid crystals provide a versatile platform due to their ability to host topological defects with well‐defined optical and mechanical properties. Here, we introduce a field‐induced nematodynamic templating strategy to program liquid crystal coatings prior to photopolymerization. Resonant standing waves generate large‐area lattices of topological defects that are permanently encoded into a polymer network with high fidelity. The resulting coatings exhibit defect‐specific surface topographies that are reversibly tunable with temperature, while preserving their ability to generate optical vortices and enabling thermally controlled phase and spectral responses. These results demonstrate that topological defects act as programmable units coupling optical and mechanical functionalities within a single platform. Beyond optics, the approach further enables spatial functionalization through guided incorporation of fluorescent particles, highlighting its potential for multifunctional coatings. This defect‐encoded and field‐programmable strategy provides a scalable route toward reconfigurable flat optics, adaptive surfaces, and sensing platforms.