Suicidal thinking, self-harm and suicidal acts are common, although determining their precise prevalence is complex. Epidemiological work has identified a number of associated demographic and clinical factors, though, with the exception of past acts of self-harm, these are non-specific and weak future predictors. There is a critical need shift focus from managing ‘suicidality-by-proxy’ through general mental health treatments, to better understand the neuropsychology and neurophysiology of such behaviour to guide targeted interventions. The model of the cognitive control of emotion (MCCE) offers such a paradigm, with an underlying pan-diagnostic pathophysiology of a hypoactive prefrontal cortex failing to suitably inhibit an overactive threat-responding limbic system. The result is a phenotype – from any number of causative gene-environment interactions – primed to impulsively self-harm. We argue that such neural dysconnectivity is open to potential therapeutic modification from repetitive transcranial magnetic stimulation (rTMS). The current evidence base for this is undoubtedly extremely limited, but the societal and clinical burden self-harm and suicide pose warrants such investigation.