The authors examined the relation between smoking status and fruit and vegetable (FV) consumption among a population-based sample and examined differences in psychosocial factors that may influence diet and inform intervention efforts. The authors recruited adults (N = 2,540) from 5 US health plans to participate in a Web-based dietary intervention trial. At baseline, smokers ate fewer FV servings per day (p < .001) and were less likely to meet the 5 A Day goal (p < .001). Smokers reported lower self-efficacy, overall motivation, and intrinsic motivation for meeting daily FV recommendations. Fewer smokers expected that eating 5 FV servings a day would reduce their risk for diabetes (p = .02) or obesity (p = .008). Smokers are an important target group for dietary intervention. Intervention efforts should attempt to increase smokers' motivation and confidence in their abilities to change their eating patterns and educate them about the health benefits of eating FV.