Recent studies have shown that graphene-derived materials not only feature outstanding multifunctional properties, but also act as model materials to implant nanoscale structural engineering insights into their macroscopic performance optimization. In this work, we explore strengthening and toughening strategies of this class of materials by introducing multimodal crosslinks, including long, strong and short, self-healable ones. We identify two failure modes by fracturing functionalized graphene sheets or their crosslinks, and the role of brick-and-mortar hierarchy in mechanical enhancement. Theoretical analysis and atomistic simulation results show that multimodal crosslinks synergistically transfer tensile load to enhance the strength, whereas reversible rupture and formation of healable crosslinks improve the toughness. These findings lay the ground for future development of high-performance paper-, fiber- or film-like macroscopic materials from low-dimensional structures with engineerable interfaces.