A facile method of preparing highly folded cross-Linked polymeric microparticles has been developed via one-pot suspension polymerization under high-speed homogenization. The wrinkles result from the evaporation of solvent in the crosslinked microparticles. The effects of rnicroparticle cross-linking density and solvent on the polymer have been studied in detail. It was found that a medium cross-linking density (DVB/St = 0.5 by weight) is optimal for producing the most folded surface and the higher the solvent content, the deeper the surface wrinkles. This method is very simple and in principle can be applied to produce wrinkled microparticles with other chemical compositions.