Exploring stable cycling electrode materials with high energy and power density is the key to accelerating the development and application of supercapacitors. Ti3C2Tx, which is the most investigated member of the family of two‐dimensional layered transition‐metal carbides, has attracted considerable attention, owing to its unique two‐dimensional morphology, large interlayer spacing, outstanding metallic conductivity, abundant chemical surface, and ultrahigh volumetric capacitance. However, the inherent restacking tendency of ultrathin Ti3C2Tx sheets hinder its practical application. In this review, the synthetic methods and charge‐storage mechanisms of Ti3C2Tx are stressed to provide clues for improving its electrochemical performance. Functionalization, including architectural construction, hybridization, and surface modification of the Ti3C2Tx sheets, to circumvent difficulties and application in supercapacitors is then summarized. Accordingly, the aim is to highlight the opportunities and challenges for Ti3C2Tx‐based materials in practical applications in supercapacitors.