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Grafting with poly­(N-vinyl-2-pyrrolidone) (PVP) was used to functionalize silica. The functionalized silicas were characterized by scanning electron microscopy, nitrogen adsorption, energy-dispersive X-ray analysis, Fourier transform spectroscopy, and thermogravimetric analysis. The Barrett–Joyner–Halenda analysis confirmed that PVP-modified silica samples have a mesoporous structure. Bovine serum albumin (BSA) was immobilized onto the surface of PVP-modified silica systems through physical adsorption. Also it was shown that the adsorption capacity of the tested samples depends on the quantity of PVP inside the silica matrix, which confirmed the formation of a specific complex between BSA and PVP. In addition, the effects of pH, time, and concentration on BSA adsorption were investigated. The maximum BSA adsorption capacity was 71.54 ± 2.0 mg/g. The desorption and reusability of all prepared samples were studied as well. PVP-modified silicas are capable of holding more BSA compared to nonmodified silica. These characteristics indicate that PVP-modified silicas have great potential for efficient protein encapsulation.