Negative affect (e.g., depression) is associated with accelerated age-related cognitive decline and heightened dementia risk. Fewer studies examine positive psychosocial factors (e.g., emotional support, self-efficacy) in cognitive aging. Preliminary reports suggest that these variables predict slower cognitive decline independent of negative affect. No reports have examined these factors in a single model to determine which best relate to cognition. Data from 482 individuals 55 and older came from the normative sample for the NIH Toolbox for the Assessment of Neurological and Behavioral Function. Negative and positive psychosocial factors, executive functioning, working memory, processing speed, and episodic memory were measured with the NIH Toolbox Emotion and Cognition modules. Confirmatory factor analysis and structural equation modeling characterized independent relations between psychosocial factors and cognition. Psychosocial variables loaded onto negative and positive factors. Independent of education, negative affect and health status, greater emotional support was associated with better task-switching and processing speed. Greater self-efficacy was associated with better working memory. Negative affect was not independently associated with any cognitive variables. Findings support the conceptual distinctness of negative and positive psychosocial factors in older adults. Emotional support and self-efficacy may be more closely tied to cognition than other psychosocial variables. (JINS, 2014, 20, 1–9)