Background: Lung cancer with intracranial metastasis requires concurrent treatment of the primary lung tumor and the secondary brain tumor. This study aimed to investigate the short-term clinical efficacy of concurrent bronchial artery and posterior inferior cerebellar artery microcatheter interventional chemotherapy for the treatment of adenocarcinoma of the lung with solitary cerebellar metastasis. Material/Methods: Seventeen patients with adenocarcinoma of the lung with solitary cerebellar metastasis received concurrent microcatheter interventional chemotherapy via the bronchial artery and posterior inferior cerebellar artery. Two cycles of treatment with teniposide (VM-26), carmustine (BCNU), carboplatin (CBP), and pirarubicin (THP) were performed every four weeks. Results: Four patients (23.53%) achieved a complete response (CR), five patients (29.41%) achieved a partial response (PR), seven patients (41.18%) had stable disease (SD), and only one patient (5.88%) developed progressive disease (PD). The objective response rate (ORR) and disease control rate (DCR) were 52.94% (9/17) and 94.12% (16/17), respectively. Four patients (11.76%) developed grade 1/2 chemotherapy toxicity, which included three cases (8.82%) of gastrointestinal toxicity and one case (2.84%) of granulocytopenia, but no grade 3/4 toxicity was found. During microcatheter interventional chemotherapy, three patients (8.82%) developed intracranial complications, including two cases (5.88%) of cerebrovascular spasm and one case (2.94%) of cerebral edema. Conclusions: In 17 patients with adenocarcinoma of the lung with solitary cerebellar metastasis, concurrent microcatheter interventional chemotherapy via the bronchial artery and posterior inferior cerebellar artery was safe and showed short-term efficacy.