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RATIONALE AND OBJECTIVES To evaluate the method and effectiveness of Angio-CT-guided transcatheter arterial chemoembolization (TACE) immediately in combination with radiofrequency ablation (RFA) in the treatment of large hepatocellular carcinomas (HCCs; maximum enhancing diameter >5 cm). MATERIALS AND METHODS A retrospective analysis was conducted on 48 patients with solitary large HCCs who were admitted from October 2012 to June 2016 and treated by immediate combination therapy, and 48 patients with solitary large HCCs who were treated by a sequential combination (RFA at 2-4 weeks after TACE) therapy in the same period were randomly selected as controls. After treatment, the success rates of the immediately combined technique, the short-term outcomes of the immediately combined treatment (using the modified response evaluation criteria in solid tumor standard), and the survival rates were evaluated. RESULTS The success rate of the immediately combined technique was 100%. The complete remission rates 1, 3, and 6 months after treatment in the study group were 58.3%༌56.2%, and 47.9%, respectively, while the corresponding complete remission rates of control group were 37.5%, 33.3%, and 27.1%, respectively. The 1-, 2-, and 3-year survival rates of the study group were 95.8%, 85.4%, and 58.3%, respectively, while the corresponding survival rates of the control group were 83.3%, 68.7%, and 43.8%, respectively. None of the patients had any serious complications. CONCLUSION Angio-CT-guided TACE immediately in combination with RFA is a feasible, safe method for the treatment of large HCCs with excellent short-term outcomes and improved long-term prognoses.