Given the negative consequences of the ongoing COVID-19 pandemic on public health, his study aimed at investigating: (1) the differences between adults with and without chronic illness in buying behavior, vaccination intention, pandemic worry, and the health belief model (HBM) components; (2) the HBM components as mediators of the relationship between pandemic worry and vaccination intention. The sample consisted of 864 adults (66.6% females, Mage = 47.61, SD = 9.23), of which 20.5% reported having a chronic illness. Associations between pandemic worry, vaccination intention, and HBM were ascertained using correlation and mediation analyses. Individuals with chronic illness reported a higher level of pandemic worry, higher levels of perceived threat, greater benefits from vaccination, had lower self-efficacy and bought more medicine and sanitary/hygienic products. No significant differences were observed regarding vaccination intention, barriers against vaccination, and changes in food buying behavior. We found that the relationship between pandemic worry and vaccination intention was partially mediated by the perceived threat of disease and the benefits of vaccination. Pandemic worry predicted vaccination intention directly but also through the contribution of the perceived threat of disease and the benefits of vaccination. These findings suggest that presenting evidence of COVID-19 vaccine efficacy and the benefits of having the vaccine (especially for vulnerable groups, such as chronic illness patients) will encourage the population to follow vaccination recommendations.