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Poor cardiorespiratory fitness and low physical activity have been identified as determinants of greater arterial stiffness, a mechanism that can partially explain the association of both variables with increased cardiovascular disease. However, the nature of these associations are not clear because cardiorespiratory fitness and physical activity can both mediate and confound the associations of one another with arterial stiffness. This issue was therefore examined in a population-based cohort of young adults. Subjects included 405 young men and women participating in an ongoing longitudinal study, the Northern Ireland Young Hearts Project. Pulse wave velocity was used to determine arterial stiffness in 2 arterial segments (aortoiliac and aortodorsalis pedis) using a noninvasive optical method. Cardiovascular fitness was estimated with a submaximal cycle test of physical work capacity and physical activity was estimated using a modified Baecke questionnaire. Associations were investigated with the use of multiple linear regression models with adjustment for potential confounders and/or intermediate variables. Cardiorespiratory fitness and sports-related physical activity (but not leisure- and work-related physical activity) were inversely associated with arterial stiffness in young adults. The associations between sports-related physical activity and arterial stiffness were strongly mediated by cardiorespiratory fitness, whereas physical activity levels did not disturb the associations between cardiopulmonary fitness and arterial stiffness. These findings suggest that arterial stiffness-related benefits of exercise are most likely to accrue if exercise prescription in young adults targets improvements in cardiorespiratory fitness.