Collagen is a promising biomaterial for drug delivery due to advantages including high biocompatibility and biodegradable property. However, transforming collagen into solid nanoparticles is difficult, although the solid dosage form is advantageous for some administration routes including pulmonary and oral drug delivery. In this study, collagen solid nanoparticles are prepared in one-step using electrospray deposition under ambient temperature and pressure conditions. Although collagen molecules formed micron-sized aggregates in acetic acid solutions spontaneously, electrospraying the collagen solutions resulted in formation of nanofibers. Solid nanoparticles were obtained by increasing conductivity of the solution and/or inducing structural perturbation of the collagen molecules using salts. The ability of solid collagen particles as a drug carrier was demonstrated by incorporating theophylline as a model drug using a coaxial spray technique. Release of theophylline was controlled by cross-linking collagen molecules. Electrospray deposition was proved to be a powerful method for producing solid collagen nanoparticles for drug delivery.