To address the aggravating energy and environment issues, the cheap, highly active, and durable electrocatalysts as noble metal substitutes both at the anode and cathode are actively pursued. Among them, heteroatom-doped graphene-based materials show extraordinary electrocatalytic performance, some even close to or outperforming the state-of-the-art noble metals such as Pt and IrO 2 -based materials. This review provides a concise appraisal on graphene doping methods, the possible doping configurations and their unique electrochemical properties, including single-and double-doping with N, B, S, and P. In addition, heteroatom-doped graphene-based materials are reviewed as electrocatalysts for oxygen reduction (ORR), hydrogen evolution (HER), and oxygen evolution reactions (OER) in terms of their electrocatalytic mechanisms and performance. Significantly, three-dimensional (3D) heteroatom-doped graphene structures have been discussed, especially those that can be directly utilized as catalyst electrodes without extra binders and supports.