The two-dimensional structure, ultrahigh mechanical performance, and remarkable self-lubricating behavior of few layers of graphene (bilayers or trilayers) make them a wise choice as second-phase materials to enhance the mechanical and tribological properties of the coating. In this research, the goal is to fabricate a simultaneously exfoliated graphene-reinforced Cr3C2NiCr composite coating using shroud plasma spraying. The mechanical properties, such as hardness, elastic modulus, and fracture toughness of the 2 wt % reinforced coating, were improved by 70.4, 31.8, and 61.5%, respectively. These enhancements are attributed to the uniform dispersion, crack bridging, and crack arrest mechanisms facilitated by exfoliated graphene within the matrix. Furthermore, the wear volume loss, wear rate, and coefficient of friction of the coating decreased by 55.7, 55.7, and 78.7%, respectively. The enhancement in tribological properties is attributed to the high hardness and super lubricating behavior of exfoliated graphene. The findings highlight the potential of exfoliated graphene in advancing the performance of composite coatings for various industrial applications.