This study presents a detailed and comprehensive investigation into the macro-scale performance, strength gain mechanisms, environment and economic performance of graphene oxide (GO)-enhanced low-emission concrete. A comprehensive experimental program evaluated fresh and hardened properties, including slump retention, bleeding, air content, compressive, flexural, and tensile strength, drying shrinkage, and elastic modulus. Scanning Electron Microscopy (SEM), energy-dispersive spectroscopy (EDS), Thermogravimetric analysis (TGA) and proton nuclear magnetic resonance (¹H-NMR) was employed to examine microstructural evolution and early age water retention, confirming GO’s role in accelerating cement hydration and promoting C-S-H formation. Optimal performance was achieved at 0.05% GO (by binder weight), resulting in a 25% increase in 28-day compressive strength without compromising workability. This outcome is attributed to a tailored, non-invasive mixing strategy, wherein GO was pre-dispersed during synthesis and subsequently blended without the use of invasive mixing methods such as high shear mixing or ultrasonication. Fourier-transform infrared (FTIR) spectroscopy further validated the chemical compatibility of GO and PCE and confirmed the compatibility and efficiency of the admixture. Sustainability metrics, including embodied carbon and strength-normalized cost indices (USD/MPa), indicated that, although GO increased material cost, the overall cost-performance ratio remained competitive at breakeven GO prices. Enhanced efficiency also led to lower net embodied CO₂ emissions. By integrating mechanical, microstructural, and environmental analyses, this study demonstrates GO’s multifunctional benefits and provides a robust basis for its industrial implementation in sustainable infrastructure.

Graphene oxide (GO) has been widely reported to enhance the mechanical performance of cementitious composites. However, the fundamental hydration mechanisms underlying these improvements, such as GO’s role as a nucleation site, remain poorly explored and quantified. This study presents a comprehensive, non-destructive investigation into the time-dependent hydration behaviour of GO-induced cement pastes using time-domain ¹H Nuclear Magnetic Resonance (NMR) spectroscopy, supported by thermogravimetric analysis (TGA), humidity-controlled water-retention tests, and compressive strength tests. Cementitious composites containing 0.035%, 0.065%, and 0.08% GO by weight of cement (bwoc) were monitored from 4 h to 28 days to track the evolution of discrete water phases, including capillary, inter-hydrate, gel pore, and interlayer water. NMR results reveal that GO initially facilitates water redistribution by retaining free water within its layered structure, followed by a delayed but sustained release that promotes continued hydration and a progressive shift toward less mobile pore–water environments at later curing ages. TGA confirms enhanced formation of hydration products in GO-induced cementitious systems, with an optimal dosage of 0.035% bwoc achieving the most sustained hydration and highest compressive strength. Higher GO dosages accelerate early hydration but limit later-stage hydration due to diffusion barriers formed by hydration products. This study provides time-dependent scientific evidence of GO’s dual role as a hydration nucleation agent and water-release regulator, establishing a mechanistic basis for dosage optimization in nano-engineered cementitious composites.