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Summary The endeavors to develop manufacturing methods that can enhance polymer and composite structures in spacecraft have led to much research and innovation over many decades. However, the thermal stability, intrinsic material stress, and anisotropic substrate properties pose significant challenges and inhibit the use of previously proposed solutions under extreme space environment. Here, we overcome these issues by developing a custom-designed, plasma-enhanced cross-linked poly(p-xylylene):diamond-like carbon superlattice material that enables enhanced mechanical coupling with the soft polymeric and composite materials, which in turn can be applied to large 3D engineering structures. The superlattice structure developed forms an integral part with the substrate and results in a space qualifiable carbon-fiber-reinforced polymer featuring 10–20 times greater resistance to cracking without affecting the stiffness of dimensionally stable structures. This innovation paves the way for the next generation of advanced ultra-stable composites for upcoming optical and radar instrument space programs and advanced engineering applications.