The synthesis of ammonia (NH3) from nitrogen (N2) under ambient conditions is of great significance but hindered by the lack of highly efficient catalysts. By performing first-principles calculations, we have investigated the feasibility for employing a transition metal (TM) atom, supported on Ti3C2T2 MXene with O/OH terminations, as a single-atom catalyst (SAC) for electrochemical nitrogen reduction. The potential catalytic performance of TM single atoms is evaluated by their adsorption behavior on the MXene, together with their ability to bind N2 and to desorb NH3 molecules. Of importance, the OH terminations on Ti3C2T2 MXene can effectively enhance the N2 adsorption and decrease the NH3 adsorption for single atoms. Based on proposed criteria for promising SACs, our calculations further demonstrate that the Ni/Ti3C2O0.19(OH)1.81 exhibits reasonable thermodynamics and kinetics toward electrochemical nitrogen reduction.