Understanding the nanoscale friction properties of 2D materials and further manipulating their friction behaviors is of great significance for the development of various micro/nanodevices. Recent studies, taking advantage of the close relationship between friction and surface charges, use an external out‐of‐plane electric field to control the interfacial friction. Nevertheless, friction increases with the application of the out‐of‐plane electric field in most cases. Here, an in‐plane potential gradient is applied for the investigation of the contribution of electric charges to friction on the surfaces of 2D materials. Experimental results show that the friction between an atomic force microscope tip and the flakes of 2D materials decreases with the application of the in‐plane potential gradient, and the higher the potential gradient, the greater the friction decrease. By comparing the in situ atomic‐level stick‐slip maps before and after the application of the in‐plane potential gradient, it is proposed that the promotion of low friction dissipative motion during the stick‐slip process owing to the presence of the potential gradient gives rise to the friction reduction. These results not only help to reveal the origin of friction, but also provide a novel way to manipulate friction through an electrically‐controlled sliding process.