In the present study, biopolymeric coatings of polyhydroxybutyrate (PHB) were deposited on 316L stainless steel substrates. The PHB coatings were developed using the spin coating method. To improve the adhesion of the PHB coating on the substrate, this method uses an atmospheric plasma treatment. Adhesion tests show a 156% increase in adhesion after 5 s of surface treatment. Raman spectroscopy analysis of the polymer shows the incorporation of functional groups and the formation of new hydrogen bonds, which can help us bind drugs and promote osteogenesis after plasma treatment. Additionally, the electrochemical behaviors in artificial body fluids (Hanks’ solution) of the PHB coatings on the steel were evaluated with potentiodynamic tests, which revealed a decrease in the corrosion current and resistance to the transfer of the charge from the electrolyte to the 316L steel because of the PHB coating. All the PHB coatings were characterized using scanning electron microscopy and Raman spectroscopy after the electrochemical tests. This analysis confirmed the diffusion of electrolyte species toward the surface and the degradation of the polymer chain for the first 15 s of treatment with atmospheric plasma. These findings support the claim that plasma surface modification is a quick, environmentally friendly, and cost-effective method to enhance the performance of PHB coatings on 316L stainless steel for medical devices.