Nanoscale energy harvester holds promise for the development of self-powered nanosystems, while molecular self-assembly of bio-inspired materials has attracted much research effort in recent years. Here we report the controlled growth of vertically aligned FF peptide microrods and their application in nanogenerators. The peptide has recently been demonstrated as a sustainable and smart material for piezoelectric energy conversion. Utilizing both piezoelectric and triboelectric effects is of significant research interest due to their complementary energy conversion mechanisms. We discovered a simple and efficient approach to integrate the piezoelectric nanogenerator with triboelectric nanogenerator. The stacking one layer atop the piezoelectric peptide-based nanogenerator to form the single-electrode triboelectric nanogenerator eliminate the needed extra electrode and complicated connection found in other devices. The energy conversion process is simplified and improved. This work demonstrated the first biomaterial-based hybrid nanogenerator and significantly advanced the study of smart biomaterials. Our work can enable new applications of bio-inspired materials in areas such as energy harvesting and storage, electromechanical sensing and actuation, drug delivery, as well as fundamental studies of FF-based structures.