The internal phosphorus (P) pollution is a major cause of water eutrophication. Although the traditional powders materials, with good performance, were difficult to recycle due to its shape, and the reaction mechanism between materials and internal P was rarely elucidated. In this work, a hydrotalcite composite material (MgFe-LDHs hybrid gel microspheres) was prepared via chemical crosslinking to eliminate internal P pollution both in overlying water and sediments effectively. Benefiting from the strong coordination between iron hydroxide on the MgFe-LDHs surface and internal P, the P adsorption capacity was up to 1256.38 mg/kg under natural conditions, the IP (NaOH-P and HCl-P) and OP were 78 % and 22 %, respectively. During 40-days remediation experiment, with the addition of MgFe-LDHs hybrid gel microspheres, whatever in the mixed or the capped, promoted a conversion from stable P to soluble active P of NaOH-P in sediments, and thus contributing to an easy adsorption of NaOH-P by MgFe-LDHs hybrid gel microspheres (The NaOH-P in sediments decreased by 16 % and 22 %, respectively). Meanwhile, the excessive stable HCl-P (only a minor portion) that could not be adsorbed by MgFe-LDHs remained in the form of Ca-P in sediments. Additionally, the MgFe-LDHs hybrid gel microspheres improved the microbial community structure, and the microorganism was involved in the elimination of internal P simultaneously. In summary, this study proposed a promising remediation approach to resolve the problem of internal P pollution in eutrophic water with high efficiency, cost-effective, and environmentally friendly.