The nanoindentation response of graphene (Gr) coating on nanotwin titanium-aluminum (nt-TiAl) matrix composites was studied using molecular dynamics (MD) simulation. The indentation velocity, twin boundary spacing, and parallel and vertical Z-axes are studied. The results show that the bearing capacity and hardness of Gr coating is significantly higher than that after coating failure, and the load-displacement curve shows the same phenomenon. Damage to the substrate material at varying speeds is indicated by atomic aggregation near the Gr coating, with the center of aggregation showing a negative correlation with indentation velocity. The matrix's damaged area is larger when the twin layer is perpendicular to the Z-axis and deeper when parallel, showing that the twin structure limits material damage by hindering dislocation expansion. Moreover, the presence of Gr coating delayed the matrix's plastic deformation process. This delay effect significantly improves the mechanical properties of composites, which have potential applications in aerospace.