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We still have little understanding of short-term predictors of suicidal thoughts and behaviors (STBs). Prior research links increased negative affect to STBs, but the vast majority of earlier work is limited by measuring negative affect at one time point and aiming to predict STBs months or years in the future. Recently, intensive longitudinal studies have shown that negative affect is associated with suicidal thoughts over relatively short, clinically useful time periods; however, the specific patterns and types of negative affect that predict STBs remain unclear. Using ecological momentary assessment (EMA) data from psychiatric inpatients hospitalized for suicide risk (n = 83), this study sought to test whether the patterns (means and variability) of two types of negative affect (anxiety/agitation and shame/self-hatred, which were derived from a larger EMA battery) during hospitalization predict STBs in the 4 weeks after discharge: an extremely high-risk time for suicidal behavior. The mean—but not the variability—of both anxiety/agitation and shame/self-hatred during hospitalization predicted the number of days with suicidal thoughts after discharge. The mean and the variability of shame/self-hatred—but not anxiety/agitation—predicted post-discharge suicide attempt. We discuss implications for assessment and treatment of suicidal individuals and propose key directions for future research. SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s42761-021-00058-6.