Objectives To investigate the correlation between sarcopenia and arterial stiffness in Caucasians, centering on the relationship between skeletal mass index (SMI) and the cardio‐ankle vascular index (CAVI) to assess the use of CAVI in predicting sarcopenia. Design Cross‐sectional Setting United Kingdom. Participants UK adults aged 45 years and over (N = 366, n = 177 male, n = 189 female). Measurements Bioimpedance analysis was used to derive SMI. CAVI score was calculated using a vascular screening system. Handgrip strength was measured using a standard dynamometer. Results Average CAVI was significantly correlated with SMI (correlation coefficient (r) = −0.285, p < .001), with higher correlation in women (r = −0.416, p < .001) than men (r = −0.214, p = .01). CAVI had the highest correlation with SMI from appendicular muscle (fat‐free mass in men, r = −0.253, p = .002; predicted muscle mass in women, r = −0.436, p < .001). There was a significant difference in average CAVI between groups, with participants who were not sarcopenic having lower CAVI (8.98) than those who were sarcopenic (9.80) (p < .001, t‐test). Linear regression was performed using SMI as the dependent variable. After adjustment for age, average CAVI was a significant predictor of SMI in women (beta = −0.332, p < .001) but not men. Conclusion Indices of sarcopenia are independently associated with a higher CAVI, with greater correlation in women than men. The CAVI can be used to assess overall vascular compliance and may be a useful operator‐independent tool that can be used to measure sarcopenia and its cardiovascular implications in older adults. J Am Geriatr Soc 67:317–322, 2019.