Liquid crystal microcapsules have attracted increasing attention due to their sophisticated structures and adjustable multifunctional features. However, the synthesis of a microscale substrate with wide electromagnetic waveband modulation characteristics and good photoelectric stabilization is still limited and challenging. Herein, a new breed of microcapsules containing dye-doped liquid crystals in a yolk-shell configuration with VTES (vinyl-trim-ethyl-silane)-modified FeO@SiO is created. It exhibits an unexpected color enhancement effect, reversible electrochromic performance, and excellent magnetically controllable characteristics. Additionally, a multispectral (visible light, near-infrared light, and high-frequency electromagnetic wave) electro-responsive fabric based on the proposed microcapsules was developed to explore its application in wearable sensors. The present work opens an avenue toward the fabrication of microscale microencapsulated soft materials with a continuous and stable yolk-shell structure. Moreover, it will expand the application regimes of liquid crystal materials in smart windows and advanced textiles.
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