Bioelectrochemical　systems　(BESs)　exhibit　great　potential　for　simultaneous　wastewater　treatment　and　energy　recovery.　However,　the　efficiency　of　microbial　electrocatalysis　is　fundamentally　limited　by　the　high　resistance　and　poor　biocompatibility　of　electrode　materials.　Herein,　we　construct　a　novel　＂binder-free＂　3D　biocompatible　bioelectrode　consists　of　1D　aminated　carbon　nanotubes　(CNTs-NH2)　and　2D　conductive　reduced　graphene　oxide　(rGO)　nanosheets　through　one-step　electrodeposition.　As　expected,　the　maximum　current　density　reached　to　3.25 ± 0.03 mA cm-2　with　the　rGO@CNTs-NH2　electrode,　which　is　4.33-fold　higher　than　that　of　a　bare　rGO　(0.75 ± 0.01 mA cm-2),　and　is　among　the　best　performance　reported　for　three-dimensional　electrodes.　The　high　microbial　electrocatalytic　activity　is　mainly　attributed　to　the　excellent　performance　of　electron　transfer　and　bacterial　colonization,　which　originates　from　the　3D　interconnecting　scaffold,　fast　1D　CNTs　＂e-bridge＂　and　positively　charged　surface.