Catalytic CO2conversion to renewable fuel is of utmost importance to establish a carbon-neutral society. Bioelectrochemical CO2reduction, in which a solid cathode interfaces with CO2-reducing bacteria, represents a promising approach for renewable and sustainable fuel production. The rational design of biocatalysts in the biohybrid system is imperative to effectively reduce CO2into valuable chemicals. Here, we introduce methanol adapted Sporomusa ovata(S. ovata) to enhance the slow metabolic activity of wild-type microorganisms to our semiconductive silicon nanowires (Si NWs) array for efficient CO2reduction. The adapted whole-cell catalysts enable an enhancement of CO2fixation with a superior faradaic efficiency on the poised Si NWs cathode. The synergy of the high-surface-area cathode and the adapted strain achieves a CO2-reducing current density of 0.88 ± 0.11 mA/cm2, which is 2.4-fold higher than the wild-type strain. This new generation of biohybrids using adapted S. ovataalso decreases the charge transfer resistance at the cathodic interface and facilitates the faster charge transfer from the solid electrode to bacteria.