In the present paper, thermosensitive coatings are prepared by deposition of P(NIPAM-co-AAc) microgel particles on precoated silicon wafers. The effect of pH, substrate precoating, and preparation technique is studied. The pH value is found to significantly influence the adsorption density, while the substrate surface charge is less important. Hence, the electrostatic contribution of the particle-particle interaction seems to play a more pronounced role for the adsorption density than at least the electrostatic part of the particle-surface interaction. For the latter, also nonelectrostatic contributions like hydrogen bonding and surface roughness play an important role. Immersion of the prepared polyelectrolyte/microgel layers in buffers leads to a reorganization of the adsorbed particles at the surface.