Individuals with serious mental disorders (SMD) may have a higher risk of vitamin D (VIT-D) deficiency. They also experience higher mortality because of coronavirus disease 2019 (COVID-19) infection. Therefore, we have conducted a comprehensive review to examine the significance of VIT-D for public health and public mental health during the ongoing COVID-19 pandemic. This review had three specific aims, from a global perspective to (a) create a profile of VIT-D and review the epidemiology of VIT-D deficiency, (b) explore VIT-D deficiency as risk factor for SMD and COVID-19 infections and (c) examine the effectiveness of VIT-D supplementation for both conditions. We found that, in terms of SMD, the evidence from laboratory and observational studies points towards some association between VIT-D deficiency and depression or schizophrenia. Mendelian randomisation studies, however, suggest no, or reverse, causality. The evidence from intervention studies is conflicting. Concerning COVID-19 infection, on proof of principle, VIT-D could provide a plausible defence against the infection itself and against an adverse clinical course. But data from observational studies and the first preliminary intervention studies remain conflicting, with stronger evidence that VIT-D may mitigate the clinical course of COVID-19 infection rather than the risk of infection in the first place. From a public health and public mental health point of view, based on the currently limited knowledge, for individuals with SMD, the benefits of VIT-D optimisation through supplementation seem to outweigh the risks. VIT-D supplementation, however, should not substitute for vaccination or medical care for COVID-19 infection.