AbstractThere is a current need to fabricate new biobased functional materials. Bottom‐up approaches to assemble simple molecular units have shown promise for biomaterial fabrication due to their tunability and versatility for the incorporation of functionalities. Herein, the fabrication of catalytic protein thin films by the entrapment of catalase into protein films composed of a scaffolding protein is demonstrated. Extensive structural and functional characterization of the films provide evidence of the structural integrity, order, stability, catalytic activity, and reusability of the biocatalytic materials. Finally, these functional biomaterials are coupled with piezoelectric disks to fabricate a second generation of bio‐inorganic generators. These devices are capable of producing electricity from renewable fuels through catalase‐driven gas production that mechanically stimulates the piezoelectric material.