Suicide is a significant public health problem, with incidence rates and lethality continuing to increase yearly. Given the large human and financial cost of suicide worldwide alongside the lack of progress in suicide prediction, more research is needed to inform suicide prevention and intervention efforts. This study approaches suicide from the lens of suicide note-leaving behavior, which can provide important information on predictors of suicide. Specifically, this study adds to the existing literature on note-leaving by examining history of suicidality, mental health problems, and their interaction in predicting suicide note-leaving, in addition to demographic predictors of note-leaving examined in previous research using data from the National Violent Death Reporting System (NVDRS, n = 98,515). We fit a logistic regression model predicting leaving a suicide note or not, the results of which indicated that those with mental health problems or a history of suicidality were more likely to leave a suicide note than those without such histories, and those with both mental health problems and a history of suicidality were most likely to leave a suicide note. These findings reinforce the need to tailor suicide prevention efforts toward identifying and targeting higher risk populations.