Ti-6Al-4V is widely used in the aviation industry because of its high strength, and good heat resistance. However, severe tool wear on the rake face occurs during the milling of Ti-6Al-4V, which is caused by intense friction between the tool rake face and the chips. To investigate tool wear in the milling of Ti-6Al-4V, ultrasonic vibration is introduced, and a cutting force prediction model that considers tool-chip contact interface friction behavior in Ultrasonic Longitudinal-Torsional Vibration-Assisted Milling (ULTVAM) is proposed in this paper. First, the tool tip motion trajectory and dynamic cutting thickness under ULTVAM were analyzed calculated, and compared with those in Common Milling (CM). Subsequently, the effects of ultrasonic vibration on the shear force under the ultrasonic softening effect, the friction force, and the friction reversal force on the tool-chip contact interface were investigated. A dynamic milling force model under ULTVAM was established before and after friction force reversal caused by ultrasonic longitudinal-torsional vibration. Finally, numerous experiments were conducted to validate the proposed model, and the experimental results indicated that the calculated dynamic milling forces agreed well with the measured values, with errors in the X and Y directions of 5.51% and 10.23%, respectively. In addition, the average roughness of the workpiece surface also decreased (1.08, 0.9, 0.6, 0.7 μm under ultrasonic amplitudes of 0, 1, 2, and 3 μm) and the tool wear state improved on the rake face under ULTVAM.