LAUSR

Mesoporous carbon microparticles (MCMPs) with anisotropic shapes and ordered structures are attractive materials that remain challenging to access. In this study, a facile yet versatile route is developed to prepare anisotropic MCMPs by combining neutral interface‐guided 3D confined self‐assembly (3D‐CSA) of block copolymer (BCP) with a self‐templated direct carbonization strategy. This route enables pre‐engineering BCP into microparticles with oblate shape and hexagonal packing cylindrical mesostructures, followed by selective crosslinking and decorating of their continuous phase with functional species (such as platinum nanoparticles, Pt NPs) via in situ growth. To realize uniform in situ growth, a “guest exchange” strategy is proposed to make room for functional species and a pre‐crosslinking strategy is developed to preserve the structural stability of preformed BCP microparticles during infiltration. Finally, Pt NP‐loaded MCMPs are derived from the continuous phase of BCP microparticles through selective self‐templated direct carbonization without using any external carbon source. This study introduces an effective concept to obtain functional species‐loaded and N‐doped MCMPs with oblate shape and almost hexagonal structure (p6mm), which would find important applications in fuel cells, separation, and heterogeneous catalysis.