In this work, the preparation and characterization of films based on polysulfone (PSF) filled with zinc oxide, ZnO, nanoparticles (NPs) are conducted. The novelty of this research mainly relies on two points: (i) the use of a commercial airbrush to prepare or modify materials, and (ii) the design of new materials (nanocomposites) for the consolidation and restoration of historical bones. To accomplish these objectives, free-standing thin films and ancient bone coatings of PSF/ZnO nanocomposites with different particle contents (0%, 1%, 2%, 5% and 10%, % wt) are prepared using a commercial airbrush. Mechanical characterization is carried out to correlate properties between free-standing thin films and coatings, thus understanding the final performance of the coatings as consolidants for ancient bones. Thin films of PSF/ZnO show that the elastic modulus (E) increases with particle content. The mechanical behavior of the surfaces of the treated and untreated bones is studied locally using Martens hardness measurements. Maximum values of Martens hardness are obtained for the bone samples treated with polysulfone filled with 1% ZnO nanoparticles (HM = 850 N·mm−2) or 2% ZnO (HM = 625 N·mm−2) compared to those treated just with neat PSF (HM = 282 N·mm−2) or untreated bone (HM = 140 N·mm−2), indicating there is a correspondence between rigidity of free-standing films and hardness of the corresponding coatings. In terms of mechanical performance, it is demonstrated the existence of a balance between nanoparticle concentration and probability of nanoparticle aggregation, which allows better material design for ancient bones consolidation.