Gelatin remains one of the most important biopolymeric material platforms because of its availability, safety, biocompatibility, biodegradability, and stimuli-responsive properties. Here we report a simple, rapid, and reagentless anodic deposition method to assemble gelatin hydrogels from aqueous salt solutions onto an electrode surface. Results indicate that anodic reactions partially oxidize gelatin to yield a covalently cross-linked network that can perform multiple functions. First, anodically deposited gelatin remains activated, allowing covalent protein grafting and thus enabling biofunctionalization for electrochemical biosensing. Second, the gelatin retains its thermally responsive physical cross-linking properties that enable switching functions. Finally, the physical and chemical cross linking mechanisms are reversible, which enables self-healing functions. Thus, anodic deposition provides a facile method to assemble gelatin-based multifunctional matrices for diverse applications in bioelectronics.