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Developing reticular reinforcement and heterogeneous microstructure remains persistent challenges in one-dimensional carbon nanotube (CNT)-Cu system. We herein fabricated dual-heterostructured Cu composite by diazotizing CNT into cross-linked (CL) networks and achieving bimodal grain distribution. The CL-CNT networks uniformly dispersed in Cu matrix, forming strong C–N/O–Cu covalent bonds at the interfaces and effectively retarding grain growth to create ultra-fine grain (UFG) regions around them. The CL-CNT networks/UFG regions, along with the surrounding coarse grain (CG) regions, resulted in a remarkable synergy between mechanical and electrical properties within the composite. Systematic analysis indicates that CL-CNT network acts as a whole to bear loading, remarkably enhances the load-transfer strengthening and promotes the dislocation accumulation around the interface. Meanwhile, hetero-deformation between “hard” CL-CNT networks/UFG regions and “soft” CG regions lead to extra-strengthening and hardening associated with strain partitioning, generation of geometrically necessary dislocation (GND) and strain delocalization. In-situ tensile test further reveals that CL-CNT/Cu with dual-heterostructure introduces the extra-toughening via crack bridging and deflection mechanisms. Besides, CL-CNT network with the robust interface is considered to reduce the interfacial inelastic scattering and provide additional paths for electron transport, accounting for the high electrical conductivity. This work highlights the importance of configuration design of reinforcement in tailoring heterostructured metal matrix composites (MMCs) with outstanding comprehensive performance.