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Efficient load transmission between concrete and steel reinforcement by bonding action is a key factor in the process of the design procedure of bar-reinforced concrete structures. To enhance the bond strength of steel/concrete composites, the impact of graphene nanoplatelets (GnP) on the bond stress and bond stress–slip response of deformed reinforcement bars, embedded in high-performance concrete (HPC), was investigated using bar pullout tests. In the current study, 36 samples were produced and examined. The main variables were the percentages of GnP, the steel reinforcement bar diameter, and embedded length. Bond behavior, failure mode, and bond stress-slip response were studied. Based on the experimental findings, the inclusion of GnP had a significant favorable influence on the bar-matrix interactions due to the bridging action of GnP as a nano reinforcement. For 0.02 wt.% of GnP, the bond strength was enhanced by more than 41.28% and 53.90% for steel bar diameters of 10 and 16 mm, respectively. The HPC-GnP mixture displayed a reduction in the initial slippage in comparison to the control sample. The test findings were compared to the prediction models created by other researchers and the ACI 408R-12 code.