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Simple Summary: Currently, as a neoadjuvant conversion therapy (NCT), pazopanib combined with neoadjuvant chemoradiotherapy could improve the pathological response of unresectable soft tissue sarcoma (uSTS). However, there is no available evidence of its effectiveness with respect to tumor reduction and surgical margins. In China, anlotinib is a novel tyrosine kinase inhibitor (TKI) that is approved for STS. In this study, adding anlotinib to adriamycin and ifosfamide resulted in an increased rate of tumor regression, surgical conversion and R0 resection in patients with uSTS, particularly for synovial sarcoma and liposarcoma. Severe toxicities are more frequent than monotherapy, but they are controllable. (1) Background: This study investigated the safety and efficiency of adriamycin and ifosfamide combined with anlotinib (AI/AN) as a neoadjuvant conversion therapy in uSTS. (2) Methods: Patients with uSTS were eligible to receive AI/An, including adriamycin (20 mg/m2/d) and ifosfamide (3 g/m2/d) for the first to the third day combined with anlotinib (12 mg/d) for 2 weeks on/1 week off, all of which combine to comprise one cycle. Surgery was recommended after four cycles of treatment. (3) Results: A total of 28 patients were enrolled from June 2018 to December 2020. The best tumor responses included eight patients with partial responses and 20 with a stable disease. Patients with synovial sarcoma and liposarcoma had a significant decrease in the number of tumors compared with fibrosarcoma (p = 0.012; p = 0.042). The overall response rate and disease control rate were 28.57% and 100%, respectively. In total, 24 patients received surgery, while the rates of limb salvage and R0 resection were 91.67% (n = 22/24) and 87.50% (n = 21/24), respectively. Until the last follow-up visit, the mean PFS and RFS were 21.70 and 23.97 months, respectively. During drug administration, 67.87% of patients had grade ≥3 AEs. No treatment-related death occurred. (4) Conclusions: AI/AN followed by surgery showed favorable efficiency and manageable safety in patients with uSTS. A randomized controlled study with a large cohort should be performed for further investigations. [ABSTRACT FROM AUTHOR]