Background: Tobacco is a major cause of cardiovascular disease, and current treatments lack long-term efficacy. Promoting physical activity may be a viable population-level approach to improving cardiovascular health among smokers. Purpose: To characterize smokers engaging in any physical activity based on demographics, quitting behaviors, health perceptions, preventive health behaviors, and disease status to identify targets for subsequent intervention. Methods: A national sample of smokers participating in the Health Information National Trends Survey (HINTS) 4 Cycle 2 data collection (N = 491) was analyzed using bivariate and multivariate regression models to characterize smokers engaging in any physical activity. Results: Some past-week physical activity was reported by 62% of smokers. "Active" status was associated with being younger (Exp(B) = 0.971; P < 0.001), lower body mass index (Exp(B) = 0.955; P = 0.011), fewer hours of daily screen time (Exp(B) = 0.903; P = 0.001), consuming at least one cup of fruit and vegetables daily (Exp(B) = 1.971; P = 0.005), and non-consideration of a quit attempt (Exp(B) = 0.606; P = 0.021). Discussion: Smokers participating in any physical activity also demonstrated a more healthful cardiovascular risk profile, suggesting that promoting physical activity in completely inactive smokers could improve overall cardiovascular health. Translation to Health Education Practice: Use of a multiple health behavior change approach to promote physical activity and related behaviors in smokers holds promise for improving cardiovascular health.