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Abstract Inspired by the brilliant and tunable structural colors based on the large refractive index contrast (Δn) and non‐close‐packing structures of chameleon skins, ZnS–silica photonic crystals (PCs) with highly saturated and adjustable colors are fabricated. Due to the large Δn and non‐close‐packing structure, ZnS–silica PCs show 1) intense reflectance (maximal: 90%), wide photonic bandgaps, and large peak areas, 2.6–7.6, 1.6, and 4.0 times higher than those of silica PCs, respectively; 2) tunable colors by simply adjusting the volume fraction of particles with the same size, more convenient than the conventional way of altering particle sizes; and 3) a relatively low threshold of PC's thickness (57 µm) possessing maximal reflectance compared to that (>200 µm) of the silica PCs. Benefiting from the core–shell structure of the particles, various derived photonic superstructures are fabricated by co‐assembling ZnS–silica and silica particles into PCs or by selectively etching silica or ZnS of ZnS–silica/silica and ZnS–silica PCs. A new information encryption technique is developed based on the unique reversible “disorder–order” switch of water‐responsive photonic superstructures. Additionally, ZnS–silica PCs are ideal candidates for enhancing fluorescence (approximately tenfold), approximately six times higher than that of silica PC.