Damage initiation due to the interfacial debonding plays a vital role in the mechanical properties of graphene-reinforced concrete. In this research, multi-scale modeling is exploited to study the effect of volume fraction, aspect ratio, and interaction properties of the multi-layer graphene nanoplatelets (GNPs) on the mechanical properties of reinforced concrete, assuming perfectly bonded and cohesively bonded interaction between the contact surface of the matrix and the GNPs. The cohesive zone model has been used to observe the debonding behavior and damage initiation between the concrete matrix and nanocomposites for cohesively bonded interaction. The required cohesive zone parameters were estimated based on the previously calculated information on graphene–graphene interactions. The results show that by increasing the volume fraction and aspect ratio of GNP, nanofiller improves the mechanical properties of the nanocomposite. In addition, results reveal that interaction properties significantly affect the mechanical properties of graphene-reinforced concrete.