This paper presents research about the embedding and release of gentamicin from an electrochemical deposition of polypyrrole from ionic liquids such as choline chloride on TiZr bioalloy. The electrodeposited films were morphologically investigated using scanning electron microscopy (SEM) with an EDX module, and polypyrrole and gentamicin were both identified using structural FT-IR analysis. The film’s characterization was completed with an evaluation of hydrophilic–hydrophobic balance, with electrochemical stability measurements in PBS and with antibacterial inhibition. A decrease in the value of the contact angle was observed from 47.06° in the case of the uncoated sample to 8.63° in the case of the sample covered with PPy and GS. Additionally, an improvement in the anticorrosive properties of the coating was observed by increasing the efficiency to 87.23% in the case of TiZr–PPy–GS. A kinetic study of drug release was performed as well. The drug molecule might be provided by the PPy–GS coatings for up to 144 h. The highest amount released was calculated to be 90% of the entire drug reservoir capacity, demonstrating the effectiveness of the coatings. A non-Fickian behavior was established as a mechanism for the release profiles of the gentamicin from the polymer layer.