This study reports a simple sequential micromolding method to produce monodisperse anisotropic microparticles with precisely controllable patchy size and chemistry of compartmentalization. Specifically, our fabrication procedure involves sequential formation of primary and secondary compartments in micromolds via surface tension-induced droplet formation coupled with simple photopolymerization. We demonstrate the capability of sequential micromolding technique by generating Mickey mouse-shaped particles with precisely controllable patchy size and chemistry of compartment and the fabrication method needs no sophisticated control or expensive facilities. The micromolding technique applied in this study can control the size of patchy diameter from 15 to 31 μm by simply adjusting the concentration of photocurable monomer in ethanol. Finally, the Mickey mouse-shaped microparticles with negatively charged patches are confirmed by selective binding of positively charged fluorescence dyes. These results prove a simple, robust, and scalable fabrication of highly monodisperse and complex anisotropic microparticles in a controlled manner based on sequential micromolding.