Instantaneous Mechanical Programming of Polymer Microparticle Shape and Surface Architecture

ABSTRACT Structurally anisotropic polymer microparticles with controlled surface topographies are essential for applications in self‐assembly, interfacial engineering, and responsive materials. However, practical methods for fabricating such complex morphologies remain limited. Here, we demonstrate an instantaneous mechanically driven strategy for simultaneously programming particle shape and surface architecture through a refined rubbing process. By optimizing particle plasticization, pressure distribution, and stress transmission, spherical polymer particles were transformed into cylindrical particles within only 10 s. Patterned silicon substrates enabled direct mechanical transfer of periodic surface structures, while variations in substrate topology and deformation pathway produced diverse anisotropic architectures. This simple mechanically driven process provides a straightforward platform for programming hierarchical polymer microparticle architectures.