The effectiveness of using modified Mg-Fe hydrotalcite to separate cerium from binary nitric acid solutions that represent possible abundance of cerium and europium in different natural and artificial sources is studied. Within this context, hydrotalcite is modified using bis (2,4,4-trimethylpentyl) phosphinic acid (Cyanex 272). Structural investigations indicated that Cyanex is incorporated into hydrotalcite structure by bonding with Fe. The material is chemically stable in different solutions conditions. Separation process applicability was investigated using multi-variant analysis, the results show that the material could be used efficiently to separate cerium from binary leaching solutions similar to that of natural resources. Cerium recovery from the material was assessed by investigating different eluents of different concentrations, optimum recovery was obtained using 1 M HCl at 0.2 concentration factor and cerium could be recovered from loaded material within 3 cycles. Solutions speciation and loaded material spectroscopic results indicated that Ce species are exchanged with Fe+3 and H+ in hydrotalcite and Cyanex. Sorption equilibrium data analysis for binary and single leaching solutions indicated the heterogeneous nature of the separation sites and confirmed that the process is chemical and part of the separation is done mainly on multilayer sites. Transient separation and recovery behaviors were investigated; the reactions follow pseudo second order and boundary layers play important role in controlling the separation kinetics. Transient recovery follow Langmuir-Freundlich modified regular solution kinetics model (LF-mRSK), where local affinity coefficient in case of HCl is larger than that in case of Citirc. (C) 2017 Elsevier B.V. All rights reserved.