The effect of particles' kinetic energy and particle-substrate relative hardness ratio on anchor layer formation during aerosol deposition (AD) were investigated in this work. Fast anchor layer formation was observed using a substrate with a low relative hardness ratio (copper) while alumina fragments were generated using high relative hardness ratio substrates (alumina and sapphire). Using a room temperature AD method, novel formation of nanocomposite films exhibiting optical properties control was demonstrated. The desired nanocomposite particles were first formed by a facile electrostatic adsorption method prior to AD. Optical transmittance in the ultra-violet (UV) and infra-red (IR) regions could be controlled using the nanocomposite films while exhibiting good transmittance in the visible region. The feasibility of this nanocomposites thick film formation at room temperature would be beneficial for the development of optical-related nanocomposite ceramic films.