Suicidal behaviour poses a major challenge to clinicians and health policy makers due to its difficult prediction and prevention, and its substantial impact at individual and societal levels. Although current research focuses particularly on the biological causes of suicidal behaviour, surprisingly little use has been made of structural and functional neuroimaging in order to increase our understanding of the suicidal brain. This chapter reviews the few available studies that have utilized functional neuroimaging, including brain perfusion and receptor ligand studies. The results of these studies have contributed to the development of the suicidal brain concept. The suicidal brain is thought to be composed of the frontotemporal cortex (in connection with the hippocampus) and the prefrontal cortex (in conjunction with the amygdala). These structures appear to be involved in the social cognitive and behavioural expressive components of the suicidal brain. Evidence is increasingly showing, among others using functional neuroimaging techniques, that these two components are involved in the neurobiologically mediated basic neuropsychological dysfunctions associated with suicidal behaviour.