Microbial Electrosynthesis Microbial electrosynthesis holds the promise of sustainable chemical production. In article number 2203480, Guillermo C. Bazan and co-workers show that 3D living biocomposites integrating electroactive bacteria with an n-type conjugated polyelectrolyte allow efficient long-range electron transfer from electrode to living cells, thereby enabling microbial electrosynthesis. The one-step self-assembly process offers a simple and effective strategy to improve bioelectrochemical systems.