This study introduces a novel and sustainable method of producing graphene from coconut shells and investigates its application in Graphene, Ni/Graphene, and Zn/Graphene electrodes for advanced energy storage devices. The graphene was synthesized scalably using a pyrolysis and impregnation technique, with its successful synthesis verified by X-ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDX), and electrical conductivity measurements characterizations. The study highlights the enhanced performance of Zn/Graphene electrodes, which outperform both pure graphene and Ni/Graphene variants. This superior performance is attributed to the smaller particle size of Zn (mean = 2.356 µm) compared to Ni (mean = 3.09 µm), and Zn’s more favorable electron configuration for electron transfer. These findings demonstrate the potential of bio-derived graphene composites as efficient, high-performance electrodes, paving the way for more sustainable and cost-effective energy storage solutions.