This study aimed to develop a longitudinal ultrasonic-assisted milling system to investigate the machinability of titanium (Ti) Alloy Ti-6Al-4V (TC4). Aiming at reduced milling force and enhanced surface quality, ultrasonic-assisted milling was investigated taking into account the following processing parameters: spindle speed (cutting rate) n, feed per tooth fz, milling depth ap, and ultrasonic amplitude A. A comparison was made with conventional milling. The results of univariate tests demonstrated that the ultrasonic amplitude had the most significant impact on the milling force along the z-axis, resulting in a reduction of 15.48% compared with conventional milling. The range analysis results of multivariate tests demonstrated that ap and fz were the dominant factors influencing the cutting force. The minimum reduction in the milling force in ultrasonic-assisted milling along the x-, y-, and z-axes was 11.77%, 15.52%, and 17.66%, respectively, compared with that in conventional milling. The ultrasonic-assisted milling led to reduced surface roughness and enhanced surface quality; the maximum surface roughness in ultrasonic-assisted milling was 25.93%, 36.36% and 26.32% in terms of n, fz, and ap, respectively. In longitudinal ultrasonic-assisted milling, the periodic “separation-contact” was accompanied by microimpacts, resulting in even smaller intermittent periodic cutting forces. Hence, regular fish scale machining mesh was observed on the processed surface, and the workpiece surface exhibited high cleanness and smoothness. The reasonable configuration of ultrasonic-assisted milling parameters can effectively improve the milling force and surface quality of Ti alloys and accumulate reference data for the subsequent machining process research.