Vanadium titanomagnetite (VTM) is an important mineral for developing titanium resources, but the comprehensive recovery of ilmenite separation is extremely poor, resulting in the low-efficiency utilization of titanium resources. Here, the separation of ilmenite from VTM ore is studied by combining magnetic separation and flotation technologies. In particular, the floatability of mixed MOH/PG-1 collectors is thoroughly investigated. The results show that a concentrate with a TiO2 grade of 9.90% can be separated via weak magnetic separation and coarse particle tailing dumping. The concentrate grade is then increased to 14.32% via strong magnetic separation and floating separation of sulfur minerals. Finally, a TiO2 grade of 46.34% is obtained through closed-circuit flotation using mixed MOH/PG-1 collectors. The mixed collectors are very efficient and can enhance the chemical adsorption of the Ti4+, Fe3+, and Fe2+ ions in the ilmenite concentrate compared with the MOH collector, thereby increasing the TiO2 grade and recovery by 3.31% and 1.20%, respectively. This is beneficial for improving the comprehensive utilization of titanium resources in VTM ores.