To prepare alpha zirconium phosphate (α-ZrP) with high interlayer distance, grafting ratio and thermal stability, 1,2-epoxypropane was used to modify α-ZrP as the epoxy group reacting with P-OH on the external and internal surfaces of α-ZrP to form P-O-C bonds after small amines pre-intercalation. Different characterization techniques were used, including X-ray Powder Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FT-IR), Thermo-Gravimetric Analysis (TGA) and Carbon Mass Nuclear Magnetic Resonance (13C MAS NMR). The results of XRD confirmed the pre-intercalation of amino-propane and the intercalation of 1,2-epoxypropane, as the interlayer distance increased from 7.5 Å to 16.9 Å and 15.3 Å, respectively. FT-IR and 13C MAS NMR results confirmed the formation of P-O-C bonds between 1,2-epoxypropane and α-ZrP. TGA analysis showed that the grafting ratio of 1,2-epoxypropane was 19.44%.