A sense of control and autonomy are key components in guiding health-related behaviors and quality of life in people with chronic diseases. This study investigated whether autonomy support from health professionals moderates the impact of personal control on psychological well-being through healthy behaviors in patients with hypertension and cardiovascular comorbidities. Data from 149 hypertensive patients with comorbid cardiovascular risk factors were collected via self-administered surveys. A moderated mediation effect of a hypothesized model was analyzed using the PROCESS macro bootstrapping method. Autonomy support from health professionals moderated the relationship between personal control and healthy behaviors (B = 0.16, t = 2.48, p < 0.05), showing that the effect of personal control on healthy behaviors differed by the level of autonomy support. Additionally, autonomy support moderated the mediation effect of healthy behaviors in the relationship between personal control and psychological well-being (Index = 0.15; 95% CI = 0.010, 0.335). The mediation effect existed only in patients with higher autonomy support. The findings demonstrate that autonomy support from health professionals plays a crucial role in reinforcing the positive impact of personal control on healthy behaviors and psychological well-being. Enhancing the supportive attitudes of health professionals that facilitate patients’ autonomous self-regulation is necessary for better health outcomes in people with combined cardiovascular diseases.