Liquid crystals (LC), when combined with photolithography, enable synthesis of microparticles with 2D and 3D shapes and internal complexities. Films of nematic LCs are prepared using mixtures of reactive (RM257) and non-reactive mesogens with controlled alignment of LCs at the confining surfaces, photo-polymerized the RM257 using a photomask, and then extracted the unreacted mesogens to yield the polymeric microparticles. The extraction results in a controlled anisotropic shrinkage amount dependent on the RM257 content and the direction dependent on LC alignment. Control over the aspect ratio, size, and thickness of the microparticles are obtained with a coefficient of variance less than 2%. In addition, non-parallel LC anchoring at the two surfaces results in a controllable right- or left-handed twisting of microparticles. These methods may find substantial use in applications including drug delivery, emulsions, separations, and sensors, besides their potential in revealing new fundamental concepts in self-assembly and colloidal interactions.