The modulation of surface properties of Ti3C2Tx plays a crucial role in its diverse applications across various fields. However, a straightforward and reliable technique for controlling its surface functional groups remains elusive. In this study, we achieved controlled modification of Ti3C2Tx surface functional groups using atmospheric‐pressure cold plasma. We evaluated the plasma generation characteristics and found that the gas parameters could influence the discharge power and lead to different gas temperatures with the same voltage. Spectral analysis confirmed the presence of numerous reactive species in the plasma, facilitating the breaking and recombination of chemical bonds of functional groups on the Ti3C2Tx surface. The interaction between the plasma jet and Ti3C2Tx film revealed that the semiconductor properties of the Ti3C2Tx film limit the plasma diffusion area, while N2 doping and increased gas flow rates respectively reduce and enlarge the coverage area of cold plasma. A brief one‐minute cold plasma treatment induced a slight etching effect on the Ti3C2Tx film surface, effectively altering the ‐O and ‐F functional groups. However, it is noteworthy that excessive cold plasma treatment in the air may result in partial oxidation of Ti3C2Tx, necessitating the use of custom gas environments in further applications. This research provides valuable insights into surface modification techniques for Ti3C2Tx with potential implications in a wide range of applications.