This study presents the enhanced performance characteristics of Portland Pozzolana Fly ash-based cement composites (PPC) reinforced by Graphene Oxide (GO) a super Nano-material. In this study, GO was reinforced at 0.02%, 0.04%, 0.06%, 0.08%, and 0.1% by weight of cement to PPC to investigate the effects of GO addition and to check their performance enhancement. Characterization techniques such as Nuclear Magnetic Resonance (NMR), Field Emission Scanning Electron Microscopy (FESEM), Scanning Electron Microscopy (SEM), Energy Dispersive X-ray Spectroscopy (EDAX), Fourier-transform Infrared spectroscopy (FTIR), X-ray Diffraction (XRD), Thermogravimetric Analysis (TGA), and Differential Thermogravimetric (DTG) studies were investigated to check the properties of synthesized GO and 28 days of hydrated cement composites. Compared to the 28 days hydrated reference mix, 0.04% GO dosage enhanced 40.41% compressive strength in PPC composites. GO enhanced microstructural characteristics by forming rod-like and needle-like structures confirmed through SEM. The O-containing functional groups detected through FTIR in hydrated cement mortar showed GO reactivity in regulating CaCO3 precipitation at optimum dosage. Phase identification by XRD peaks showed intensities of calcite crystals which showed GO reinforcement can regulate the microstructure of PPC composites. Rich Calcium Hydrate (CH) content and bound water contents were achieved by the addition of GO at optimum dosages in PPC composites confirmed through TGA, and DTG curves. This investigation helps the addition of GO as a nano-reinforcing material which improves the overall performance of Portland cement composites. © 2021 Elsevier Ltd