Background The prospective associations between social isolation, loneliness, and health behaviors are uncertain, despite the potential importance of these relationships over time for outcomes including mortality. Purpose To examine the associations between baseline social isolation, baseline loneliness, and engagement in health behaviors over 10 years among older adults. Methods Data were from 3,392 men and women aged ≥52 years in the English Longitudinal Study of Ageing from 2004/2005 to 2014/2015. Modified Poisson regression was specified to estimate relative risks (RRs) and 95% confidence intervals for the associations between baseline social isolation, baseline loneliness, and consistent weekly moderate-to-vigorous physical activity, consistent five daily fruit and vegetable servings, daily alcohol drinking at any time point, smoking at any time point, and a consistently overweight/obese body mass index over the follow-up (all yes vs. no). Models were population weighted and adjusted for sociodemographic factors, health indicators, and depressive symptoms, with mutual adjustment for social isolation and loneliness. Results Socially isolated participants were less likely than non-isolated participants to consistently report weekly moderate-to-vigorous physical activity (RR = 0.86; 0.77-0.97) or five daily fruit and vegetable servings (RR = 0.81; 0.63-1.04). They were less likely to be consistently overweight or obese (RR = 0.86; 0.77-0.97) and more likely to smoke at any time point (RR = 1.46; 1.17-1.82). Loneliness was not associated with health behaviors or body mass index in adjusted models. Among smokers, loneliness was negatively associated with successful smoking cessation over the follow-up (RR = 0.31; 0.11-0.90). Conclusions Social isolation was associated with a range of health-related behaviors, and loneliness was associated with smoking cessation over a 10 year follow-up in older English adults.