The novel two-dimensional MXene material Ti3C2Tx boasts advantages such as large specific surface area, good electrical conductivity, and high stability, making it suitable for the field of electrocatalysis. However, Ti3C2Tx exhibits unacceptably slow kinetics during the electrocatalytic hydrogen evolution reaction (HER). Electron-metal-support interaction is an effective method for regulating the electronic state of active sites and enhancing HER performance. Therefore, in this study, Fe, Co, and Ni were respectively loaded onto Ti3C2Txvia electron beam deposition to form electron microscopy-supported interface (EMSI) effects, thereby improving the HER activity of Ti3C2Tx. The tests conclude that loading different transition metals (Fe, Co, Ni) onto Ti3C2Tx effectively enhances its HER performance. Experimental and theoretical studies further indicate that the electrocatalytic performance of Ni-loaded Ti3C2Tx is superior to that of Co-loaded and Fe-loaded Ti3C2Tx. This work presents a promising strategy for synthesizing metal-loaded MXene.