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Background: Mental well-being is an important yet often overlooked component of cardiometabolic health. Dietary habits may influence psychological outcomes, but evidence among high-risk populations in Central and Eastern Europe remains limited. This study investigated the association between dietary behaviors and mental well-being among adults with cardiometabolic risk in Hungary. Methods: A cross-sectional analysis was conducted using data from the European Health Interview Survey (EHIS) 2019. The study included 2785 adults with cardiometabolic high risk (obesity, hypertension, or hypercholesterolemia). Mental well-being was assessed using the WHO-5 Well-Being Index and categorized as poor (≤50) or better (>50). Dietary habits, sociodemographic factors, and lifestyle factors were analyzed. Weighted multivariable logistic regression was used to estimate adjusted odds ratios (ORs) and 95% confidence intervals (CIs). Results: Overall, 25.9% of participants had poor mental health. In multivariable analyses, low intake of vegetables (OR = 1.15), fruits (OR = 1.55), fruit juice (OR = 1.26), and fish (OR = 1.17), as well as inadequate water intake (OR = 1.38), were each independently associated with higher odds of poor mental health after adjustment for sex, education, income levels, self-perceived health status, physical activity, and alcohol consumption. Conclusions: Healthier dietary behaviors, particularly higher consumption of vegetables, fish, and adequate hydration, are associated with better mental well-being among individuals with cardiometabolic risk. These results underscore the need for comprehensive intervention strategies that simultaneously address physical health and psychological well-being among vulnerable populations.