Abstract: The removal and recovery of phosphorus from wastewater in an efficient and cost-effective way are critical for resolving the phosphorus crisis. The ultra-thin Ni_xFe-LDHs nanosheets with different molar ratio of Ni:Fe were fabricated by a co-precipitation method combined with ultrasonic treatment. The Zeta position and crystallinity played an important role in promoting the adsorption of LDH, which were observed in the relationship between the Zeta position, crystallinity and the molar ratio of Ni :Fe. When the molar ratio of Ni :Fe was 2 :1, the amount of phosphate adsorption could reach 248.00 mg/g. The regenerative efficiency of Ni₂Fe-LDHs was still up to 59.2% after adsorption and desorption for six cycles through proper regeneration technology.