This review investigates the association between positive psychological well-being (PPWB) and cardiovascular disease (CVD). We also consider the mechanisms by which PPWB may be linked with CVD, focusing on the health behaviors (e.g., smoking, alcohol consumption, physical activity, sleep quality and quantity, and food consumption) and biological functions (e.g., cardiovascular, inflammatory, and metabolic processes) that are most relevant for cardiovascular health. Because PPWB is a broad concept, not all aspects of PPWB may be associated with cardiovascular health. Thus, we distinguish between eudaimonic well-being, hedonic well-being, optimism, and other measures of well-being when reviewing the literature. Findings suggest that PPWB protects consistently against CVD, independently of traditional risk factors and ill-being. Specifically, optimism is most robustly associated with a reduced risk of cardiovascular events. In general, PPWB is also positively associated with restorative health behaviors and biological function and inversely associated with deteriorative health behaviors and biological function. Cardiovascular health is more consistently associated with optimism and hedonic well-being than with eudaimonic well-being, although this could be due in part to more limited evidence being available concerning eudaimonic well-being. Some similarities were also evident across different measures of PPWB, which is likely due to measurement overlap. A theoretical context for this research is provided, and suggestions for future research are given, including the need for additional prospective investigations and research that includes multiple constructs of psychological well-being and ill-being.