As the demand for uranium production-based energy worldwide has been increasing in the last decades to maintain nuclear growth for electricity production, there are great efforts towards developing an easy and inexpensive method for uranium extraction and separation from its ores. For this purpose, mesoporous inorganic cation exchangers provide an efficient separation technology that can help streamline production and lower overall cost. This study describes the development of nano-structured mesoporous sodium zirconium phosphate (NaZrP-CEX) for separation and extraction of uranyl ions from real samples. The fabricated NaZrP-CEX was well characterized by various techniques such as X-ray diffraction (XRD), Fourier Transform Infrared (FTIR), Scanning Electron Microscope (SEM), N2 adsorption/desorption, Dynamic light scattering (DLS) and zeta potential). The kinetics/thermodynamic behaviors of uranyl ion adsorption into NaZrP-CEX from an aqueous solution were minutely studied. The kinetic studies showed that the pseudo-second order model gave a better description for the uptake process. The negative value of ΔG indicate high feasibility and spontaneity of adsorption. Finally, mesoporous NaZrP-CEX can be regenerated using both of HNO3 (0.05 M) or HCl (1 M) up to seven cycles of operation.