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Highlights The realization of lightweight insulation materials is often accompanied by a decrease in ablation performance. Coordinating the contradiction between lightweight and ablation resistance is the key to the development of thermal protection technology. Addressing the need for high‐performance insulation materials within solid rocket motors (SRMs) combustion chambers, we designed three multilayer composite structural insulation materials and studied their properties. The results show that among these constructed multilayer composites, the bilayer structure exhibited the lowest density at a mere 0.72 g/cm3, marking a 27% reduction compared to the basic structure. Remarkably, the bilayer configuration demonstrated superior ablation resistance, showcasing a 25% decrease in the line ablation rate in contrast to the basic structure after oxygen‐acetylene test. This achievement embodies the successful harmonization of lightweight properties with ablation resistance. Furthermore, based on the performance and microstructure of the char layer, a further analysis revealed the enhancement mechanism of ablative performance by the multilayer composite structure. It was found that the synergistic effect of the compact/porous structure of the char layer grants the bilayer structure thermal insulation material optimal ablative performance. This work provides strong support for improving the performance of SRMs. Insulation materials with multilayer composite structures are designed. The materials exhibit both lightweight and superior ablation resistance. Compact/porous char layers enhance material ablation performance. [ABSTRACT FROM AUTHOR]