In nature, many living creatures have developed unique periodic micro-or nano-structures, well-known as photonic crystals (PC), which could interact with incident light to give rise to brilliant and non-fading structural colors for courtship, disguise, escape, and communication. [1-4] For instance, Morpho menelaus and anaxibia wings utilize the multilayer micro-concavities-based retro-reflection to exhibit bright blue and turquoise colors for mating and warning; [3,4] cephalopods possess reflecting platelets stacked in iridophores to produce iridescent colors for disguise and escape. [3,4] Inspired by these exciting natural architectures, great efforts have been devoted to developing various photonic materials with structural colors. Among them, photonic microspheres exhibit high flexibility, small size, and orientation-independent structural color because of their spherical symmetry in geometry, making them appealing for a wide range applications, including advanced photonic devices, wide viewing-angle displays, [5-9] biological sensors, [6,10-12] aesthetic pigments. [13-19] In particular, these photonic microspheres provide building blocks for constructing promising encoded patterns for complex bioassays and anti-counterfeiting, [18,20-24] and to create standalone devices for environment stimuli sensing. [23,25-27] Conventional photonic microspheres are generally crystallized from monodispersed colloidal nanoparticles (e.g., SiO 2 , polystyrene). [16,28,29] Unfortunately, the high orientation of those nanoparticles during arrangements usually causes the formation of single-crystal or multi-domain structure across the entire spherical space, resulting in non-uniform structural colors on the spherical surface. [16,21,22,28,30] A promising alternative approach for constructing photonic microspheres with uniform structural colors is to design a concentric or onion-like periodic lamellar structure like natural pearls, [26,31,32] because of its unique symmetry, fewer intrinsic defects, relatively easy prediction and control of optical properties. However, in spite of orientation-independent structural color, these concentric microspheres inevitably exhibit strong angle-dependence, which resulted from long-range ordering of the concentric lamellae in Photonic microspheres offer building units with unique topological structures and specific optical functions for diverse applications. Here, a new class of inorganic photonic microspheres with superior robustness, optical and electrical properties is reported by introducing a unique localized concentric ordering architecture and chemical interaction, which further serve as building blocks for deep pattern encoding and multiple sensory optoelectronic devices. Benefiting from localized concentric ordering architecture, the resultant photonic microspheres demonstrate orientation-and angle-independent structural colors. Notably, the formation of well-combined lamellae inorganic layers by chemical interaction grants the microspheres superior mechanical robustness, excellent so...