Total antioxidant performance (TAP) measures antioxidant capacities in both hydrophilic and lipophilic compartments of serum and interactions known to exist between them. Our objective was to assess TAP levels in a subset of Jackson Heart Study (JHS) participants and to examine associations with dietary and total (diet + supplement) intakes of alpha-tocopherol, gamma-tocopherol (diet only), beta-carotene, vitamin C, fruit, vegetables, and nuts, and serum concentrations of alpha-tocopherol, gamma-tocopherol, and beta-carotene. We conducted a cross-sectional analysis of 420 (mean age 61 y; 254 women) African American men and women participating in the Diet and Physical Activity Sub-Study of the JHS in Jackson, Mississippi. In multivariate-adjusted models, we observed positive associations between total alpha-tocopherol, total and dietary beta-carotene, and total vitamin C intakes and TAP levels (P-trend < 0.05). Positive associations were also observed for vegetable, fruit, and total fruit and vegetable intakes (P-trend < 0.05). For serum antioxidant nutrients, alpha-tocopherol but not beta-carotene was associated with serum TAP levels. There were inverse associations for serum gamma-tocopherol and TAP levels. Associations for alpha-tocopherol were seen at intake levels much higher than the current Recommended Dietary Allowance. It may, therefore, be prudent to focus on increasing consumption of fruit, vegetables, nuts, and seeds to increase total antioxidant capacity.