We investigated the association of lung function at mid-life, later in life, and its 20-year decline, with arterial stiffness later in life. We examined 5720 Atherosclerosis Risk in Communities Study participants who attended Visits 1 (1987-1989) and 5 (2011-2013). Lung function measures were forced expiratory volume in one second (FEV1) and forced vital capacity (FVC), obtained at Visits 1, 2 (1990–1992), and 5. Central artery stiffness (carotid-femoral pulse wave velocity [cfPWV]) was measured at Visit 5. We evaluated associations of lung function with later-life central artery stiffness and cfPWV >75th percentile by multivariable linear and logistic regressions. Lung function at Visit 1 (FEV1 β: −26, 95% Confidence Interval [CI]: −48, −5; FVC β: −14, 95% CI: −32, 5) and Visit 5 (FEV1 β: −22, 95% CI: −46, 2; FVC β: −18, 95% CI: −38, 2) were inversely associated with cfPWV at Visit 5, and with odds of high cfPWV in fully adjusted models. Twenty-year decline in lung function was not associated with continuous or dichotomous measures of arterial stiffness (FEV1 β: 11, 95% CI: −46, 68; FVC β: −4, 95% CI: −52, 43). Lung function at mid-life and late-life was inversely associated with arterial stiffness in later life.