Background Type 2 diabetes mellitus (T2DM) is a chronic progressive disease that significantly impacts morbidity and mortality worldwide. Glycemic control is central in diabetes management, yet complex and challenging to achieve; it can be affected by various factors. Diabetes self-care behaviors are vital strategies for effective T2DM management. Purpose To evaluate the levels of glycemic control and diabetes self-care behaviors, and the significance of each behavior on glycemic control among patients with T2DM in Jordan. Patients and Methods This cross-sectional study was conducted in medical and endocrinology outpatient clinics of three hospitals in northern Jordan. A convenience sample of 520 patients with T2DM participated in the study. Diabetes self-care behaviors, including diet, exercise, blood glucose testing, taking medication, and foot care behaviors, were measured using the Arabic version of the Summary of Diabetes Self-Care Activities (SDSCA-Arabic) questionnaire. Psychological distress was measured using the Arabic version of the 4-items Patient Health Questionnaire (PHQ-4). Glycated hemoglobin (HbA1c) levels were used to assess glycemic control. Results Out of 520 participants, 92.7% (n= 482) had poor glycemic control (HbA1c ≥7%), with a mean of 9.29% (SD=2.06) for HbA1c. The SDSCA overall mean score was 3.25 days (SD=0.88), indicating an unsatisfactory level, with 79.2% of participants having performed self-care activities 4-days/week. Greater adherence to diabetes self-care behaviors was associated with better glycemic control. Exercise was the most important predictor of HbA1c (p<0.001), followed by general diet (p<0.001), specific diet (p<0.001), and blood sugar testing (p<0.001). Moreover, the Body Mass Index (p<0.001), treatment type (p<0.001), and income (p=0.03) were significant predictors. Conclusion The proportions of poor glycemic control and unsatisfactory self-care behaviors were high among T2DM patients. To enhance patients’ self-care behaviors and lifestyles changes, the patients need tailored diabetes self-care management educational and supportive programs, conducted by qualified diabetes educators using culturally sensitive strategies.