For a long time, graphene-based nanomaterials have broad application prospects because of their excellent multi-functional properties. Here, combined with coarse-grained molecular dynamics simulations, the compressive mechanical behavior and impact resistance of graphene-assembled hollow nanospheres (GAHNs) with interlayer binders have been explored systematically. It was found that, the introduction of binders between graphene nanosheets (GNs) can effectively improve the interfacial stress-transfer, by which the compression strength and modulus can be increased by ∼ 100% and ∼ 300%, respectively, with a low content of 4.23%. Meanwhile, it is found that the role of binders is changed under different impacting velocities. When the impact velocity is small, the strong connection between layers inhibits the impact force from decomposing to neighbor graphene nanosheets, while when the velocity is high, it will help maintain the structure from being torn. The tensile-shear tests reveal the contribution of binders to stress transfer theoretically. This work provides a theoretical insight for carbon hollow spheres into the mechanical response and impact resistance under different interface situation and lays the foundation for impacting resistance application.