AbstractPetroleum-based plastics are useful but they pose a great threat to the environment and human health. It is highly desirable yet challenging to develop sustainable structural materials with excellent mechanical and thermal properties for plastic replacement. Here, inspired by nacre’s multiscale architecture, we report a simple and efficient so called “directional deforming assembly” method to manufacture high-performance structural materials with a unique combination of high strength (281 MPa), high toughness (11.5 MPa m^1/2), high stiffness (20 GPa), low coefficient of thermal expansion (7 × 10⁻⁶ K⁻¹) and good thermal stability. Based on all-natural raw materials (cellulose nanofiber and mica microplatelet), the bioinspired structural material possesses better mechanical and thermal properties than petroleum-based plastics, making it a high-performance and eco-friendly alternative structural material to substitute plastics.