Background: Physical behavior [PB, physical activity (PA), and sedentary behavior (SB)] can adjust cardiovascular mortality risk in older adults. The aim of this study was to predict cardiovascular parameters (CVPs) using 21 parameters of PB. Methods: Participants [n = 93, 73.8 (6.23) y] wore a thigh-mounted accelerometer for 7 days. Phenotype of the carotid, brachial, and popliteal arteries was conducted using ultrasound. Results: Sedentary behavior was associated with one of the 19 CVPs. Standing and light-intensity PA was associated with 3 and 1 CVP, respectively. Our prediction model suggested that an hourly increase in light-intensity PA would be negatively associated with popliteal intima-media thickness [0.09 mm (95% confidence interval, 0.15 to 0.03)]. sMVPA [moderate–vigorous PA (MVPA), accumulated in bouts <10 min] was associated with 1 CVP. 10MVPA (MVPA accumulated in bouts ≥10 min) had no associations. W50% had associations with 3 CVP. SB%, alpha, true mean PA bout, daily sum of PA bout time, and total week 10MVPA each were associated with 2 CVP. Conclusions: Patterns of PB are more robust predictors of CVP than PB (hours per day). The prediction that popliteal intima-media thickness would be negatively associated with increased standing and light-intensity PA engagement suggests that older adults could obtain health benefits without MVPA engagement.