Termination groups are exposed to the environment and can be one of the key factors determining the stability of MXenes. Although MXenes are known for rich and tunable surface chemistry, the role of termination groups in degradation processes remains poorly understood. Moreover, the rich surface chemistry of MXenes represents a significant challenge for ab-initio-based simulations due to a large combinatorial space of surface compositions. Therefore, most of the previous simulations were focused mainly on fully O-, OH-, or F-terminated MXene, which cannot be realized experimentally. Several computational studies quantified the role of termination groups in the stability of MXenes by employing ab initio thermodynamic analysis (i.e., by constructing Pourbaix diagrams and calculating defect formation energies ). These studies indicated that O-terminated MXenes are the most stable, while the presence of hydroxyl and fluorine termination groups decreases the stability, promoting the formation of Ti vacancies. More recent studies employing ab initio molecular dynamics (AIMD) simulations revealed spontaneous degradation of O-terminated surface MXenes surfaces (e.g., Ti 3 C 2 O 2 36,37 and V 2 CO 2 ) in contact with an aqueous environment. These works emphasize the need for advanced computational methods to evaluate the stability and understand the atomistic mechanism of MXene degradation.