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This study aimed to explore the relationships among Machiavellianism, theory of mind performance, and brain connectivity indicators related to both. Data came from a 3-year longitudinal cohort; analyses used 1-year follow-up data. This cohort of participants included 148 participants (mean age= 24.3) but 136 of them completed both behavioral and functional connectivity assessment. Machiavellianism was measured with the Dirty Dozen (DD12) and ToM with the Reading the Mind in the Eyes Test (RMET). Results showed that higher DD12 Machiavellianism was associated with poorer ToM performance on the RMET (ρ = −0.181, p = .028). RMET was significantly related to ToM-relevant connectivity, including positively with AC–IFG (ρ = 0.219, p = .010) and TPJ–TPJ_R (ρ = 0.190, p = .027), but negative with Precuneous–TPJ_L (ρ = −0.180, p = .036) and STG–TP (ρ = −0.189, p = .027). Importantly, Machiavellianism was linked to the same ToM-related pathways, IFG–Insula (ρ = 0.172, p = .045) and Insula–TPJ_R (ρ = −0.181, p = .035). Current results suggest that Machiavellianism and ToM may share some of the ToM circuits, especially the IFG–Insula–TPJ pathway, but the direction of their association can be further verified.