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A simple and efficient approach for the electrochemical deposition of polypeptides as bio-based covering materials for surface design is described. The method involves N-carboxyanhydride (NCA) ring-opening polymerization from its precursor to form a thiophene-functionalized polypeptide macromonomer (T-Pala), followed by electropolymerization. The obtained conducting polymer, namely polythiophene-g-polyalanine (PT-Pala), was characterized and utilized as a matrix for biomolecule attachment. The biosensing applicability of PT-Pala was also investigated by using glucose oxidase (GOx) as a model enzyme to detect glucose. The designed biosensor showed a very good linearity for 0.01–1.0 mM glucose. Finally, the antimicrobial activities of newly synthesized T-Pala and PT-Pala were also evaluated by using the disc diffusion method.