Objectives Novice meditators often struggle to recognise and intentionally disengage from self-referential thought during meditation. We investigated whether personalised high-precision neurofeedback (NF) training improves volitional disengagement from self-referential thought during meditation and enhances meditation’s outcomes. Method In a single-blind, controlled study, novices received 2 days of veridical (n = 20) or sham (n = 20) 7-T fMRI NF targeting posterior cingulate cortex (PCC) deactivation during meditation. After NF training, at-home meditation practice was monitored for 1 week, followed by an in-lab behavioural assessment. Results Both groups reported similar perceptions of NF contingency, performance, and expectancy (p > 0.05), suggesting effective participant blinding. PCC deactivation during NF-guided meditation was comparable across groups (p > 0.05). Veridical NF group showed significantly stronger negative functional coupling (d = 0.59) between PCC and dorsolateral prefrontal cortex (DLPFC), significantly greater mindful awareness (d = 0.41) and emotional well-being (d = 0.40) associated with 1-week practice, and significant correlation (r = 0.71, p < 0.01) between emotional well-being and PCC-DLPFC negative coupling. Conclusions These findings suggest that high-precision NF can improve novices’ ability to volitionally disengage from self-referential thought during meditation, thereby fostering greater mindful awareness in real-world practice and promoting emotional well-being. Preregistration This exploratory study was not preregistered.