Alterations of the sense of self induced by meditation include an increased sense of boundarylessness. In this study, we investigated behavioural and functional magnetic resonance imaging correlates of trait self-boundarylessness during resting state and the performance of two experimental tasks. We found that boundarylessness correlated with greater self-endorsement of words related to fluidity and with longer response times in a math task. Boundarylessness also correlated negatively with brain activity in the posterior cingulate cortex/precuneus during mind-wandering compared to a task targeting a minimal sense of self. Interestingly, boundarylessness showed quadratic relations to several measures. Participants reporting low or high boundarylessness, as compared to those in between, showed higher functional connectivity within the default mode network during rest, less brain activity in the medial prefrontal cortex during self-referential word processing, and less self-endorsement of words related to constancy. We relate these results to our previous findings of a quadratic relation between boundarylessness and the sense of perspectival ownership of experience. Additionally, an instruction to direct attention to the centre of experience elicited brain activation similar to that of meditation onset, including increases in anterior precentral gyrus and anterior insula and decreases in default mode network areas, for both non-meditators and experienced meditators.