The study aims to determine whether routine rehabilitation training combined with the Maitland mobilization is more effective than routine rehabilitation training alone in patients with chronic ankle instability, intending to provide a novel rehabilitation strategy for chronic ankle instability. A total of 48 subjects were divided into three groups: EG (Maitland mobilization and routine rehabilitation), CG (routine rehabilitation), and SG (sham mobilization and routine rehabilitation). The intervention was performed three times each week for 4 weeks, for a total of 12 sessions. Before and after the intervention, the muscle strength, star excursion balance test (SEBT), weight-bearing dorsiflexion range of motion (WB-DFROM), ankle range of movement, Cumberland ankle instability tool (CAIT), self-comfort visual analog scale (SCS-VAS), and self-induced stability scale (SISS-VAS) were assessed. The results showed that the improvement of SEBT, WB-DFROM, and active ankle range of movement without the pain in EG was more obvious than CG and SG, but the improvement of the self-report of ankle severity and muscle strength was not. Compared with routine rehabilitation training alone, routine rehabilitation training combined with Maitland mobilization for patients with chronic ankle instability may provide more benefit in terms of balance and ankle range of movement than routine rehabilitation alone, but the improvement in muscle strength was not evident enough.