In this study, the synthesis and experimental theoretical evaluation of a new chitosan/alginate/hydrozyapatite nanocomposite doped with Mn2 and Fe2O3 for Cr removal was reported. The physicochemical properties of the obtained materials were analyzed using the following methods: SEM-EDX, XRD, FTIR, XPS, pH drift measurements, and thermal analysis. The adsorption properties were estimated based on equilibrium and adsorption kinetics measurements. The Langmuir, Freundlich and Temkin isotherms were applied to analyze the equilibrium data. The thermodynamic analysis of adsorption isotherms was performed. A number of equations and kinetic models were used to describe the adsorption rate data, including pseudo-first (PFOE) and pseudo-second (PSOE) order kinetic equations. The obtained test results show that the synthesized biomaterial, compared to pure chitosan, is characterized by greater resistance to high temperatures. Moreover, this biomaterial had excellent adsorption properties. For the adsorption of Cr (VI), the equilibrium state was reached after 120 min, and the sorption capacity was 455.9 mg/g. In addition, DFT calculations and NCI analyses were performed to get more light on the adsorption mechanism of Cr (VI) on the prepared biocomposite.