This work reported an in-situ constructing of innovative and versatile nanotraps (NZVI/ZIF–8) namely incorporation of zero–valent iron nanoparticles (NZVI) into zeolite imidazole framework–8 (ZIF–8), and the application of the as-constructed NZVI/ZIF–8 in high efficient detoxification and imprisonment of U(VI) and Se(IV) from wastewater. The results demonstrated that controllable incorporation of NZVI with ZIF–8 used advantages of each component to generate an emphatic boosted interaction in U(VI)/Se(IV) imprisoning. The kinetic adsorption for U(VI)/Se(IV) imprisoned onto NZVI/ZIF–8 was described by pseudo-second-order model well, and the adsorption isotherms followed the Langmuir model better. Thermodynamic analysis (ΔG < 0, ΔS > 0, ΔH > 0) demonstrated that U(VI)/Se(IV) imprisoned onto NZVI/ZIF–8 was endothermic and spontaneous. XPS measurements unveiled that NZVI/ZIF–8 imprisoned U(VI)/Se(IV) by synergistic mechanism of adsorption and reduction. The N–containing functional groups on ZIF–8 was primarily responsible for adsorption, while Fe(0) and surface enriched Fe(II) from NZVI predominantly contributed to reductive conversion of U(VI)/Se(IV) into U(IV)/Se(0). In a word, ZIF-8 played an important role in imprisonment of U(VI)/Se(IV) onto the as-constructed NZVI/ZIF–8 nanotraps with intensified reactivity in comparison with naked NZVI. The findings revealed that the NZVI/ZIF–8 nanotraps would be superb scavengers towards U(VI)/Se(IV), and implied a bright future in potential application in nuclear waste management.