| Summary: | Inspired by the intelligent systems in nature, artificial systems with complicated practical functions have been developed for decades. The pathway toward the target is now based on the discoveries for new stimuli‐responsive and free‐standing materials to construct the advanced intelligent systems, instead of just electronic machines. Structural color materials, including both photonic crystalline and amorphous structures, are typical candidates due to the smart biomimetic characteristics, such as self‐healing, autonomous regulation, and on‐demand adaptability. However, to improve the stability and simplify the fabrication process of such materials, great efforts have been made in the modification of colloidal self‐assembly techniques for more efficient real‐life applications. A comprehensive review investigating various direct self‐assembly techniques of colloids for the facile fabrication of structural color materials toward practical applications is provided. Recent advances of these self‐assembly schemes of colloidal particles are presented, along with valuable design guidelines of these techniques to achieve efficient structural color materials for advanced intelligent systems.
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