Abstract Growing evidence suggests that psychological factors, such as conscientiousness and anger, as well as cognitive ability are related to mortality. Less is known about 1) the relative importance of each of these factors in predicting mortality, 2) through what social, economic, and behavioral mechanisms these factors influence mortality, and 3) how these processes unfold over long periods of time in nationally-representative samples. We use 35 years (1972–2007) of data from men (ages 20–40) in the Panel Study of Income Dynamics (PSID), a nationally representative sample in the United States, and discrete time event history analysis (n = 27,373 person-years) to examine the importance of measures of follow-through (a dimension of conscientiousness), anger, and cognitive ability in predicting mortality. We also assess the extent to which income, marriage, and smoking explain the relationship between psychological and cognitive factors with mortality. We find that while follow-through, anger, and cognitive ability are all associated with subsequent mortality when modeled separately, when they are modeled together and baseline demographic characteristics are controlled, only anger remains associated with mortality: being in the top quartile for anger is associated with a 1.57 fold increase in the risk of dying at follow-up compared with those in the bottom quartile. This relationship is robust to the inclusion of income, marriage, and smoking as mediators.