The development of simple and versatile methods for the deposition of biocompatible coatings to protect or functionalize a range of materials with different shapes is an important challenge. In this study, a versatile, room‐temperature process is presented for the deposition of silk fibroin on different materials viz., glass, polyethylene terephthalate, Ti alloy, and poly(dimethylsiloxane). Coating with thin fibroin films is achieved using an atmospheric plasma torch, wherein a silk‐fibroin aerosol solution is used as the working gas. The method consists of two sequential processes: plasma modification of the surface, followed by plasma‐assisted deposition. This allows enhanced adhesion of the protein to the underlying surfaces, and the deposition even on non‐planar and flexible substrates. The deposited films are characterized by optical microscopy, atomic force microscopy, and scanning electron microscopy. Primary and secondary structures of the surface‐attached fibroin films are investigated by Fourier transform infrared spectroscopy. The proposed approach offers a tunable and controllable strategy for the controlled deposition of proteins on complex surfaces, for a wide range of biomedical and technological applications, including dentistry and bioelectronics.

Plasma‐assisted deposition is a facile, yet sophisticated method to form biocompatible coatings on materials and introduce specific surface interactions. The plasma process provides unique features such as surface activation, functionalization, and assisted polymerization, all of which can be obtained under low power and room temperature conditions. Plasma‐assisted deposition can further provide coatings with enhanced adhesion and stability. Here, it is reported for the first time, a method for the controlled plasma deposition of the versatile biomaterial chitosan on a range of substrates – soda‐lime glass, metal alloy (Ti4Al6V), thermoplastic polymer (polyethylene terephthalate), and silicone rubber (poly(dimethylsiloxane)). The deposited chitosan films are characterized by atomic force microscopy, scanning electron microscopy and Fourier transform infrared spectroscopy, and evaluated for adhesion and stability. The proposed method is also successfully optimized for the deposition of multiple layers of different biomaterials. Specifically, coatings comprising alternate chitosan and silk fibroin layers are realized, together with patterned surfaces with programmable surface composition. The biological response of the chitosan‐on‐fibroin and fibroin‐on‐chitosan surfaces with and without patterning are investigated using cell culture experiments. Selective area deposition enables the development of improved surface finishes for biomedical devices.