While there have been tremendous studies about graphene and its applications in the past decade, so far the proposed huge potential of this material has not been materialized. One of the prerequisites to overcome these challenges is maintaining the nature and intrinsic properties of individual graphene sheets while in the state of bulk material. Thus, in this Perspective contribution, the fabrication/synthesis of the monolithic polymeric and three-dimensional (3D) cross-linked bulk materials (3DGraphene) with (doped) 2D graphene sheets as the building block will first be briefly summarized. Then, the second part will cover the redox catalytic application of these bulk materials including doped 3DGraphene, the graphene-like material polymeric C3N4 and their hybrid materials. These will include mainly oxygen reduction reactions (ORR), hydrogen evolution reactions (HER), and CO2 reduction for their latest development. Finally, challenges and outlook related to the design of 3D cross-linked graphene based materials and their catalytic applications will be briefly discussed.