Phosphorus is widely used in agriculture and industry. However, excessive phosphorus can cause eutrophication in aquatic environment. Therefore, the development of an simple, efficient and economical method for phosphate removal from wastewater is urgently needed. In this study, calcium aluminum layered double hydroxides (CaAl-LDHs) and six amino acid intercalated calcium aluminum layered double hydroxides (CaAl-amino acid-LDHs) was prepared by a facile method. In order to identify optimal amino acid, the adsorption performance of phosphate for six CaAl-amino acid-LDHs were comparatively studied. A high phosphate adsorption capacity were observed for l-Aspartic acid intercalated calcium aluminum layered double hydroxides (CaAl-Asp-LDHs). Experimental results showed that CaAl-Asp-LDHs can achieve phosphate anion adsorption capacity of 569.95 mg/g, which is significantly higher than that of CaAl-LDHs (236.86 mg/g) at pH 6.0 and favorable selectivity was observed when compared with other common anions. CaAl-Asp-LDHs exhibited a faster phosphate removal than that of CaAl-LDHs. The adsorption data of aqueous phosphate anion using CaAl-LDHs and CaAl-Asp-LDHs could be well described by the Langmuir isotherm model and pseudo-second order kinetics. Furthermore, based on the structural and morphological features, as well as fourier transform infrared spectrometer (FT-IR), diffraction of x-rays (XRD), x-ray photoelectron spectroscopy (XPS), scanning electron microscope with energy dispersive x-ray spectroscopy (SEM-EDS) and element mapping, the phosphate adsorption mechanism on CaAl-Asp-LDHs involved the electrostatic attraction, hydrogen bonds, complexation and ion exchange. Compared with the performance of other phosphate sorbents in other reported, CaAl-Asp-LDHs has the highest adsorption value. The synthesized CaAl-Asp-LDHs, therefore, would be a promising environmentally friendly material for the efficient removal of phosphate from aquatic environments.