Electrochemically active bacteria (EAB) harboring extracellular electron transfer capabilities display great potential for applications in wastewater treatment and energy recovery. However, limited biocatalytic efficiency can curtail their practical engineering applications. Building on the merits of nanomaterials (NMs) that are biocompatible with EAB, engineered nanobiohybrids that are synergistically integrated with specific bacterial components and NMs provide a novel design for engineering an advanced biocatalyst complex. In this chapter, we summarize the efficacy of NMs for their suitability in constructing nanobiohybrids. Favorable engineered nanobiohybrids attributes include high electrical conductivity, large specific surface area, desirable photocatalytic capability, stimulated production of cellular components related to electron transfer, and cytoprotection capabilities. Considering the mechanisms of interfacial electron transport and electron flux generation, the configuration of nanobiohybrids with NMs can be implemented through both endogenous and exogenous bioaugmentation, wherein nanobiohybrids are constructed at a single cell-based or biofilm-based scale with different interfacial connections. Finally, we summarize the current challenges for nanobiohybrid construction and envision the future prospects for nanobiohybrid development and applications.