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ObjectivePoor prognosis and limited treatments of liver metastases from non–small‐cell lung cancer (NSCLC) after radical surgery are critical issues. The current study aimed to evaluate the efficacy and safety of CalliSpheres® microsphere transarterial chemoembolization (CSM-TACE) plus 125I brachytherapy in these patients.MethodsA total of 23 patients with liver metastases from NSCLC after radical surgery were included. All patients received CSM-TACE 1–3 times, then 125I brachytherapy was carried out following the last CSM-TACE. Complete response (CR), objective response rate (ORR), disease control rate (DCR), survival, and adverse events were evaluated.ResultsCR, ORR and DCR were 43.5%, 87.0%, and 100%, respectively, at three months; furthermore, they were 78.3%, 100%, and 100% accordingly at six months. Moreover, most European Organization for Research and Treatment of Cancer Quality of Life Questionnaire-Core 30 (QLQ-C30) subscales of functions (including physical and emotional function) and symptoms (including pain, nausea, and vomiting) were generally improved at three months (all P < 0.05). Furthermore, median progression-free survival (PFS) was 14.0 [95% confidence interval (CI): 10.4–17.6] months, with a 1-year PFS rate of 62.9%, but the 2-year PFS rate was not reached. Moreover, the median overall survival (OS) was 22.0 (95% CI: 16.8–27.2) months, with a 1-year OS rate of 91.3% and a 2-year OS rate of 43.5%. Additionally, the main adverse events included fever (100%), pain (65.2%), liver function impairment (65.2%), fatigue (56.5%), and nausea and vomiting (52.2%), which were all categorized as grade 1–2.ConclusionCSM-TACE plus 125I brachytherapy is effective and safe in patients with liver metastases from NSCLC after radical surgery, providing a potentially optimal option in these patients.