Strontium, the main component of radioactive nuclear wastewater, is characterized by a high fission yield and an extended half-life. It is easily absorbed by the human body, thus greatly threatening the environment and the human body. In this study, a mesoporous composite phase sodium superionic conductor (NVP@NMP) was synthesized by the droplet template method, and the rapid capture of Sr2+ from wastewater was achieved by constructing a nano-heterogeneous interface to increase the ion diffusion rate. NVP@NMP showed efficient and rapid removal of strontium ions in adsorption kinetics, isothermal adsorption, solution pH, and interfering ions concentration tests. Especially the equilibrium time of 2 min for strontium absorption by NVP@NMP and a maximum theoretical adsorption capacity of 361.36 mg/g. The adsorption process was spontaneous, endothermic, and feasible. At higher concentrations of other competing ions (Na, K, Ca, Mg, and Cs), the adsorbent exhibited higher selectivity towards Sr2+.TEM, XPS, and XRD analyses revealed that ion exchange was the main mechanism for the NVP@NMP ultrafast adsorption of Sr2+. In this research, we investigated the feasibility of ultrafast strontium capture by sodium superionic conductor structured phosphates and explained the ultrafast strontium adsorption mechanism of NASICON materials through XPS.