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This study investigates the application of mesoporous aluminosilicate material with hierarchical porosity to ultralow density wood fiber composite (ULD_WFC) for improving their mechanical properties. A 300 nm thickness Si–Al inorganic film was applied to the surface of the fibers. The mesoporous aluminosilicate material with many mesopores ranging from 2 to 20 nm was obtained. Their total pore volume and Brunauer–Emmett–Teller surface area were 0.193 cm3/g and 355.2 m2/g, respectively. Thermogravimetric analysis indicated that the thermostability of ULD_WFCs was affected by Si–Al compounds. But the residual weight of ULD_WFC with Si–Al compounds was 23.87% greater than composite without Si–Al compounds. The X-ray diffraction analysis indicated partial conversion of SiO2 to α-SiC. These conditions attributed to improving the mechanical properties of ULD_WFC. The modulus of elasticity, modulus of rupture, and internal bond strength of composite with Si–Al compounds increased by 547.4%, 240.0%, and 400.0%, respectively, as compared with uncoated ULD_WFC.