摘要:SummaryBioelectrochemical systems (BESs) can fulfill the demand for renewable energy and wastewater treatment but still face significant challenges to improve their overall performance. Core efforts have been made to enhance the bioelectrode performance, yet, previous approaches are fragmented and have limited applicability, unable to flexibly adjust physicochemical and structural properties of electrodes for specific requirements in various applications. Here, we propose a facile electrode design strategy that integrates three-dimensional printing technology and functionalized modular electrode materials. A customized graphene-based electrode with hierarchical pores and functionalized components (i.e., ferric ions and magnetite nanoparticles) was fabricated. Owing to efficient mass and electron transfer, a high volumetric current density of 10,608 ± 1,036 A/m3was achieved, the highest volumetric current density with pureGeobacter sulfurreducensto date. This strategy can be readily applied to existing BESs (e.g., microbial fuel cells and microbial electrosynthesis) and provide a feasibility for practical application.Graphical abstractDisplay OmittedHighlights•A 3D-printed graphene aerogel electrode was proposed for BESs•The optimized electrode mass transfer resistance was less than 5% of carbon felt•A high volumetric current density of 10,608 ± 1,036 A/m3was achievedChemistry; Electrochemistry; Bio-electrochemistry