Development of nuclear industry has caused severe water pollution. Adsorptive removal of radionuclides from wastewater has been regarded as effective solution for environment. However, developing adsorbents with high adsorption capacity and selectivity for removal of radionuclides (such as 137Cs) is still a challenge. Herein, we adopted an in situ assemble strategy to construct a novel composite, in which zeolitic imidazolate framework (ZIF-67) was grafted into two-dimension (2D) layers of transition metal carbides/nitrides (MXenes) Ti3C2, and used it in adsorptive removal of Cs+ from wastewater. Laminated and pillaring effect of ZIF-67 increased interlayer spacing and specific surface area of Ti3C2, significantly enhancing Cs+ adsorption. MXenes matrix provided the main adsorptive sites and interaction to stabilize Cs+, while the hybrid ZIF-67 assisted adsorption. The adsorbent achieved 96.2 % removal for 5 mg·L-1 of Cs+ within 6 h, and 50.0 mg·g−1 of maximum adsorption capacity, with good recyclability for 4 times. Ion competition, kinetics and thermodynamics were studied in detail to obtain the behavior of Cs+ adsorption. Finally, adsorption mechanism was proposed that [Ti − O] − H+ and [Ti − O] groups of 2D Ti3C2 were main adsorptive sites to participate in ion exchange and complexation with Cs+, respectively, while 2-methylimidazole (2-MI) ligands in ZIF-67 were synergetic adsorption sites.