In this study, we synthesized multicomponent solid films of low-dose doxorubicin (DOX)-loaded polydimethylsiloxane (PDMS)-SiO2/CaP nanocomposites via sol–gel process combined with the method of evaporation-induced self-assembly (EISA) at low temperature. Nanomechanical properties (elasticity and adhesion) of the synthesized multicomponent films were determined by using atomic force microscopy with a PeakForce™ quantitative nanomechanical mapping imaging technique. Solid state of DOX in the synthesized films was studied by using UV–vis and fluorescence spectroscopy. The release profile of different concentrations of DOX loaded (1, 3, and 5wt%) on the multicomponent films was assessed using USP Apparatus 4 and via UV–vis end analysis. Results indicate drug–component interactions on the overall morphology of domains (size and shape), nanomechanical properties, and release behavior of the DOX-loaded nanocomposites. We observed a progressive increase in surface roughness and mean adhesive value with increasing concentration of DOX loaded (0–5wt%). In addition, for all the different concentrations of DOX-loaded, we observed a diffusion-controlled drug release.