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Purpose: To investigate clinical outcomes of drug-eluting bead transarterial chemoembolization (DEB-TACE) using HepaSpheres 20–40 µm in diameter and subsequent cisplatin-based lipiodol TACE (Cis-TACE) in patients with hepatocellular carcinoma (HCC) > 5 cm. Materials and Methods: This study included 39 consecutive patients (34 men, 5 women; mean age, 63.5 years; range, 39–80 years) who underwent DEB-TACE using HepaSpheres 20–40 µm as first-line treatment for HCC > 5 cm (mean diameter, 8.2 cm; range, 5.1–13 cm) between September 2018 and August 2019. Patients with new tumors, residual tumors, or tumor growth after initial DEB-TACE underwent subsequent Cis-TACE. Results: All 39 patients underwent initial DEB-TACE successfully, with 35 (89.7%) and three (7.7%) patients experiencing minor and major complications, respectively. After initial DEB-TACE, one patient (2.6%) achieved complete response (CR), 35 (89.7%) achieved partial response (PR), and three (7.7%) experienced progressive disease (PD). During a median follow-up period of 14.4 months (range, 0.6–23 months), 23 patients underwent Cis-TACE, with 11, three, and nine achieving CR, PR, and PD, respectively. The median overall survival time was 20.9 months (95% confidence interval (CI), 18.6–23.2 months), the median time to progression was 8.8 months (95% CI, 6.5–11.1 months), and the median time to local tumor recurrence was 16 months (95% CI, 7.4–24.6 months). Conclusions: DEB-TACE using HepaSpheres 20–40 µm in diameter can be a safe and effective initial treatment method in patients with HCC > 5 cm. Subsequent Cis-TACE constitutes a good adjuvant method to enhance tumor response after initial DEB-TACE.