In this work, the catalytic activities of Mo₂C-MXene for the co-synthesis of urea from N₂ and CO₂ are reported by well-defined density functional theory (DFT) method. The calculated results show that the presence of surface functional groups is not conducive to the CO₂/N₂ (C/N) coupling process in urea synthesis reaction. The exposed Mo₂C on the surface can realize urea synthesis at the limit point of 0.69 eV, but the large transition state energy barrier (1.50 eV) indicates that bare Mo₂C is not a promising urea catalyst. Loading single atoms can improve the urea synthesis performance of bare Mo₂C. The energy barrier of urea synthesis reaction and the transition state energy barrier of C/N coupling reaction have dropped significantly by the atomic loading of Fe and Ti on bare Mo₂C. Moreover, Ti doped Mo₂C exhibits better catalytic selectivity toward urea production, making it an excellent catalyst for urea synthesis. We hope this work can pave the way for the electrochemical synthesis of urea.