A simple and template-free method for fabrication of a modified porous graphene hydrogel electrode was developed. The method involved adding natural organic phytate in the pure graphene hydrogels. Benefiting from the introduced phosphate groups and positively charged metal ions, the flexible magnesium phytate/graphene (Mg-P/G) hydrogel electrode showed large specific capacitance of 281 F/g with a small charge transfer resistance of 0.3 . Furthermore, the flexible supercapacitor showed prominent cycling stability (about 100% retention in capacitance over 10000 cycles) and excellent mechanical flexibility (about 97.5% of its original capacitance after 500 bending cycles Graphene materials have gained considerable interest in flexible energy devices because of their unique and fascinating characteristics, especially for chemically modified graphenes (such as graphene oxide (GO) and reduced graphene oxide (rGO)).1,2 These graphene sheets also frequently have higher conductivities, much larger specific surface areas, and can be used as electrodes/active materials for flexible supercapacitor (SC).3-6 However, owing to its strong π-π stacking, rGO sheets tend to cause irreversible agglomeration or even restack to form graphite.7 Thus, the assembly and regulation of GO is a crucial factor in electrochemistry. Most research has focused on graphene-based composites with polymers, 8,9 inorganic nanoparticles, 10-12 or other carbon materials including activated carbon 13 and carbon nanotubes 14,15 to extend their functions. 3D architectures of graphene (such as graphene aerogels and hydrogels) have been frequently designed.16-20 Yet a few obstacles still need to be overcome for commercialization. For example, further improving graphene-based electrodes' mechanical flexibility, cycle stability, and searching for a safe, low-cost, renewable, and environment friendly nanomaterials to modify 3D porous graphene structures.Natural organic phytate, derived from legume seeds, cereal grains, and corn, is a nontoxic, eco-friendly, abundant, and readily available resource. 21 Phytate has six phosphate groups located symmetrically on a cyclohexane ring, which is viable for interacting with positively charged metal ions (such as Ca 2+ , Mg 2+ , Zn 2+ , etc.) and can attach to the surface of GO sheets to form a network structure through hydrogen-bond interaction.2 Based on these properties, we chose one of these positively charged metal ions (Mg 2+ ) to prepare a perforated magnesium phytate (Mg-P). The oxygen atoms in the phosphate groups and GO sheets can act as coordination atoms to chelate with metal ions (Mg 2+ ). Mg-P molecules can provide a variety of viable cross-linking sites through π-π and hydrogen-bond interaction that may "stitch" two or more GO sheets to form 3D assemblies.A major challenge in the regulation of 3D porous magnesium phytate/graphene (Mg-P/G) hydrogel requires a certain concentration and proportion of Mg-P to GO that form a stably network. Herein, we report a simple method for modifying graphene hydrogel. As e...