Graphene, as a highly promising electrode material, has garnered significant attentions due to its remarkable properties. Nevertheless, challenges persist in its commercial application in the field of energy storage and conversion, including easy stacking, inert surface and limited yield. Rational regulation of the morphology, structure and composition of graphene is demonstrated as an effective way to conquer these challenges. Herein, we adopt a facile spray pyrolysis method to achieve large-scale synthesis of 3D crumpled N, O co-doped graphene nanosheets (NO-GNs). By comprehensive characteri...