In this work, the two‐step modification process is designed to improve the dispersity and interfacial interaction of lamellar aluminum phosphate (LAP) nanoparticles (NPs). The LAP NPs are successfully modified by maleimidopropyl triethoxysilane (MPTES). LAP/blend bismaleimide (BBMI) composites were prepared by mechanical blending process. Among them, the flexural strength of the modified LAP/BBMI composites were significantly enhanced with more than 148.2 MPa, the characteristic heat resistance temperature (T40) was improved by 11.7°C, and the carbon residue rate (Y600) also increased by 8.8%. Specifically, the dielectric constant of the modified LAP/BBMI composites only display a slight enhancement, but the dielectric loss is reduced to lower than 0.015. The results are helpful to potentially apply in the fields of electromagnetic and wave transparent materials.