AbstractNatural fibers (NFs) and inorganic particles have been successfully grown in the polymer to enhance its properties. The basalt fiber (BF) and modified hydrotalcite (LDHs) reinforced epoxy resin matrix composites were prepared, and the effects of fiber and modified hydrotalcite (G‐LDHs) on the microstructural characteristics of composites were investigated. Fourier transform infrared spectroscopy and X‐ray diffraction were respectively used to analyze the structure of modified BF and G‐LDHs, and thermogravimetric analysis was performed to study thermal stability. The mechanical properties of composites, including dynamic thermomechanical and tensile and flexural properties, were respectively studied by dynamic mechanical analysis (DMA) and universal testing machine. Experimental results show the successful synthesis of high‐performance epoxy copolymers. The impact strength, tensile strength, and elastic modulus of EP/BF/G‐LDHs respectively reached 7.07 kJ/m2, 20.52 MPa, and 2595 MPa when the content ratio of BF to hydrotalcite in the additive was 3:3. The DMA test showed that the glass transition temperature (Tg) value increased by 18.3°C, and the thermal stability of composite materials was improved. The storage modulus E′ value increased by 268.04 MPa, and the stiffness of the epoxy material and the mechanical properties were also elevated. The TGA and DTG curves indicate that the cured composites also exhibit excellent thermal stability. The effect of g‐LDHS particle size on the properties of composites was also discussed. Overall, the synergistic and complementary enhancement effect of the two materials is the best when the diameter of hydrotalcite is similar to that of BF, and the performance of the composite material is considerably improved.