Arterial stiffness may be associated with cognitive function. In this study, pulse wave velocity (PWV) was measured from the carotid to femoral (CF-PWV) and from the carotid to radial (CR-PWV) with the Complior SP System (Alam Medical, Vincennes, France). Cognitive function was measured by six tests of executive function, psychomotor speed, memory, and language fluency. A total of 1433 participants were included (mean age 75 years, 43% men). Adjusting for age, sex, education, pulse rate, hemoglobin A1C, HDL cholesterol, hypertension, CVD history, smoking ,drinking, and depression symptoms, a CF-PWV > 12 m/s was associated with a lower Mini-Mental State Examination score (coefficient: −0.31, se: 0.11, p=0.005), fewer words recalled on Auditory Verbal Learning Test (coefficient: −1.10, se: 0.43, p=0.01), and lower score on the composite cognition score (coefficient: −0.10, se: 0.05, p=0.04) and marginally significantly associated with longer time to complete Trail Making Test-B (coefficient: 6.30, se: 3.41, p=0.06), CF-PWV was not associated with Trail Making Test-A, Digit Symbol Substation Test, or Verbal Fluency Test. No associations were found between CR-PWV and cognitive performance measures. Higher large artery stiffness was associated with worse cognitive function, and longitudinal studies are needed to confirm these associations.