Suicide is a serious public health problem, including among U.S. Army personnel. There is great interest in discovering objective predictors of suicide and non-fatal suicidal behaviors. The current study examined the association between neurocognitive functioning and pre-military history of suicide attempts (SA) and post-enlistment onset of SA. New Soldiers reporting for Basic Combat Training (N = 38,507) completed a comprehensive computerized neurocognitive assessment battery and self-report questionnaires. A subset of Soldiers (n = 6216) completed a follow-up survey, including assessment of lifetime SA, 3-7 years later. Six hundred eighty-nine Soldiers indicated lifetime SA at baseline and 210 Soldiers indicated new-onset SA at follow-up. Regression analyses, adjusted for demographic variables, revealed significant bivariate associations between neurocognitive performance on measures of sustained attention, impulsivity, working memory, and emotion recognition and lifetime SA at baseline. In a multivariable model including each of these measures as predictors, poorer impulse control and quicker response times on an emotion recognition measure were significantly and independently associated with increased odds of lifetime SA. A second model predicted new-onset SA at follow-up for Soldiers who did not indicate a history of SA at baseline. Poorer impulse control on a measure of sustained attention was predictive of new-onset SA. Effect sizes are small and of unlikely clinical predictive utility. We simultaneously examined multiple neurocognitive domains as predictors of SA in a large, representative sample of new Army Soldiers. Impulsivity most strongly predicted past and future SA over and beyond other implicated cognitive-emotional domains.