reducing the amount of Pt, for example, to construct hybrids electrode materials incorporating Pt-based nanocatalysts into carbon support materials, such as porous carbons, [5] carbon nanotubes (CNT), [6,7] and graphene sheets. [8] To improve the surface of chemically inert carbon materials as well as to introduce microspores, several different strategies have been investigated. A useful strategy is chemical activation by using alkali hydroxides as activating agents for pulling in microspores with narrow distribution and increasing their surface areas. [9] Another efficient strategy is heteroatom doping. Recent studies have demonstrated that it is conductive to modulate the electronic structures and chemical reactivity of carbon materials, resulting in the remarkably enhanced catalytic ability. [10] To date, a variety of heteroatom-doped carbon materials and carbon-based hybrids have been developed, such as nitrogen, phosphorus, or boron-doped carbon black, [11] carbon nanotubes, [12] or graphene, [13] nitrogen and sulfur-codoped graphene, [14] and carbon nitride-graphene hybrids. [15][16][17] It is noteworthy that incorporation of heteroatoms into the frameworks of carbon materials can help to remove the absorbed poisoning intermediates, thus ensuring the high exposure of the active sites and promoting the catalytic reaction. [18,19] In particular, graphitic carbon nitride (g-C 3 N 4 ), as a typical nitrogen-rich carbon materials, has become a hot topic of interest due to its remarkable properties including ideal 2D structure, ultrahigh nitrogen content, excellent chemical and thermal stability, which can be applied in a wide range of areas such as metalfree catalysts for water splitting, [20] CO 2 fixation, [21] organic pollutant degradation, [22] and so on.On the other hand, nanostructured materials with hierarchically multimodal pore-size distributions have become a hot topic of interest in the catalytic community owing to that they combine the micro and mesoporosity with the macroporous networks. [23] Rich mesoporosity brings large specific surface areas and the robust macropores lead to accessible diffusion pathways. 3D graphene-based frameworks, such as hydrogel, [24] aerogels, [25,26] foams, [27] and sponges, [28] are an important class of new-generation template-free hierarchically porous materials. 3D graphene-based materials are probably upgraded by the recognition that their high specific surface area and intimate A 3D hierarchically porous carbon nanocomposite constituting of graphitic carbon nitride (g-C 3 N 4 ) chemically integrated with reduced graphene oxide (rGO) via covalent CN bonds is reported. This porous nanocomposite has high nitrogen content, large surface area, interconnected porous networks, and good electrical conductivity, and is used to load Pt nanoparticles to form 3D Pt-g-C 3 N 4 -rGO catalyst for direct methanol fuel cell anode. The catalyst shows an unusual electrocatalytic ability toward methanol electrooxidation, such as high activity, intriguing poison tolerance, and rel...