The self-assembled organization of particles depends on the symmetry of their interactions, motivating the development of methods to produce nanoparticles of controlled shape and functionalization that have unique symmetry. This paper describes the use of particle adsorption to control surface modification of latex particles, and thereby produce particles with specific symmetry that assemble into desired structures. Charged polystyrene spheres were deposited as a monolayer on a polyelectrolyte film. The monolayer consisted of non-contacting particles that were present with a high degree of coverage. The particles were coated with an oppositely charged polymer layer and released from the substrate. The particle area that had been in contact with the substrate remained uncoated, resulting in patchy particles. This lithographic patch provided sufficient area to associate with other oppositely charged surfaces. Thus assemblies with complementary particles of various sizes were produced. Self-aggregation of patchy particles was found to depend strongly on the ionic strength. The size of the lithographic patch was evaluated by means of particle adsorption.