Nano-biohybrid systems that interface semiconducting nanocrystals (quantum dots, QDs) with microbial cells or proteins enable light-driven enhancement of intricate bioreactions including CO2 conversion, N2 fixation, and beyond. This complex nano-bio interface provides an opportunity to study dynamic, nanoscale electron transport and catalysis. In this thesis, we focused on 1) developing a mechanistic understanding of charge transfer at the nano-bio interface, and 2) exploring opportunities in bioinspired catalysis based on the dynamic, nanoscale control of proteins. We first developed an in-vitro bioelectronic platform that interfaced reconstituted microbial cell membranes with solution-phase QDs in an electrochemical cell. By performing cyclic voltammetry, impedance spectroscopy, and photo-chronoamperometry, we gained fundamental understanding of photochemical and diffusive subprocesses involved in interfacial, redox-mediated charge transfer. Next, we focused on charge uptake in full cells by using two-photon fluorescence lifetime imaging microscopy (FLIM) to explore charge transfer between a photoexcited QD film and microbial cells (Shewanella oneidensis) with high spatiotemporal resolution. FLIM experiments revealed rates of charge transfer at the cell-cluster length scale and demonstrated how conductive cell membrane extensions expanded the geometric footprint of charge uptake by 6-7x. Finally, inspired by the dynamic and nanoscale control over methane activation exhibited by particulate methane monooxygenase enzymes, we explored opportunities in bioinspired methane partial oxidation to methanol—a long-standing goal to address methane emissions and climate change. We found that modulating the applied potential during methane electrolysis impacts the microenvironments for methane activation, and we further discuss how controlling such microenvironments via pulsed activation may enhance methane electrocatalysis, akin to natural protein-based methane conversion.