A novel method for producing monodisperse micro- and nanosized shape memory particles from various shape memory polymers (SMPs) is reported. This method uses a polydimethylsiloxane mold to uniformly deform particles from complex shapes to other well-defined shapes, harvest them without aggressive solvents or heat, and then return them to their original shapes upon heating above a preselected trigger temperature. By manipulating the material properties of both the mold and SMP, monodisperse asymmetric particles are easily achieved. This method is demonstrated with traditional SMPs and polymers with varying degrees of reactive functionality, crystallinity, and transition temperature. This additional reactivity and the robustness of this system allow easy tailoring of the surface with click chemistry to achieve chemical asymmetry.