Food assistance recipients are at higher risk for poor cardiovascular health given their propensity to poor dietary intake and tobacco use. This study sought to evaluate the cardiovascular health status, and determine the impact of a low-intensity smoking cessation education intervention that connected mobile food pantry participants to state quit-smoking resources. A pre-post design with a 6-week follow-up was used to evaluate the impact of a 10-12 min smoking cessation education session implemented in five food pantries in Delaware. Baseline cardiovascular health, smoking behaviors and food security status were assessed. Smoking cessation knowledge, intention to quit and use of the state quit line were also assessed at follow-up. Of the 144 participants 72.3% reported having hypertension, 34.3% had diabetes, 13.9% had had a stroke. 50.0% were current smokers. The low-intensity intervention significantly increased smoking cessation knowledge but not intention to quit at follow-up. Seven percent of current smokers reported calling the quit line. Current tobacco use was five times more likely in food insecure versus food secure adults (OR 4.98; p = 0.006), even after adjustment for demographic factors. Systems based approaches to address tobacco use and cardiovascular health in low-income populations are needed. The extent to which smoking cessation could reduce food insecurity and risk for cardiovascular disease in this population warrants investigation.