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(1) Background: Cardiometabolic disease progression can be delayed if patients engage in healthy lifestyle behaviors, adherence to which is highly influenced by psychosocial factors. The present study aimed at investigating the association of self-efficacy with the adherence level to healthy lifestyle behaviors among patients with cardiometabolic diseases in Greece. (2) Methods: 1988 patients (1180 females) with cardiometabolic diseases participated. Anthropometric, demographic, socioeconomic, clinical, and lifestyle characteristics were recorded. Patients were also asked to evaluate their efficacy to comply with healthy lifestyle behaviors. (3) Results: The majority exhibited unhealthy lifestyle behaviors. A subgroup demonstrated elevated self-efficacy in maintaining healthy habits despite facing diverse psychosocial challenges. Individuals with higher educational attainment, socioeconomic status, and rural/semi-urban residency had significantly elevated self-efficacy. Those with heightened self-efficacy exhibited significantly lower BMI and reduced prevalence of certain health conditions. Self-efficacy significantly influenced adherence to the Mediterranean diet, physical activity engagement, and smoking cessation, even in challenging circumstances. (4) Conclusions: This study represented an innovative approach in examining the role of self-efficacy in shaping health behaviors and outcomes within a Greek population. By integrating specific psychosocial circumstances into the analysis, valuable insights were provided into the contextual factors influencing self-efficacy and adherence to healthy lifestyle behaviors. [ABSTRACT FROM AUTHOR]