Modulating the temporoparietal junction (TPJ), especially the right counterpart, shows promises in enhancing social cognitive ability. However, it is ambiguous whether the functional lateralization of TPJ determines people's responsiveness to brain stimulation. Here, this issue is investigated with an individual difference approach. Forty‐five participants attended three sessions of transcranial direct current stimulation (tDCS) experiments and one neuroimaging session. The results support the symmetric mechanism of left and right TPJ stimulation. First, the left and right TPJ stimulation effect are comparable in the group‐level analysis. Second, the individual‐level analysis reveals that a less right‐lateralized TPJ is associated with a higher level of responsiveness. Participants could be classified into positive responders showing cognitive enhancement and negative responders showing cognitive impairment due to stimulation. The positive responders show weaker connectivity between bilateral TPJ and the medial prefrontal cortex, which mediates the prediction of offline responsiveness by the lateralization and the social‐related trait. These findings call for a better characterization and predictive models for whom tDCS should be used for, and highlight the necessity and feasibility of prestimulation screening.