NiFe layered double hydroxide (LDH) currently are the most efficient catalysts for the oxygen evolution reaction (OER) in alkaline environments. However, the development of high-performance low cost OER electrocatalysts using straightforward strategies remains a significant challenge. In this study, we describe an innovative microbial mineralization-based method for in situ-induced preparation of NiFe LDH nanosheets loaded on nickel foam and demonstrate that this material serves as an efficient oxygen evolution electrocatalyst. In the microbial mineralization process, bacteria adhere to electrode materials and promote the surface nucleation of nanomaterials when metal ions are present. Specifically, our findings indicate that biomineralization accelerates the formation and regulation of NiFe LDH. The new electrocatalyst displays excellent OER performance, with a small overpotential of 220 mV at 10 mA cm