Due to the characteristics of high strength, high chemical activity and low heat conduction, titanium alloy materials are generally difficult to machine. As a typical titanium alloy with higher strength and lower heat conductivity, the machinability of titanium alloy TC21 is very poor and its cutting process is companied with larger cutting force and rapid tool wear. Straight-tooth milling tool is often used to cut the groove and side surface in the titanium alloy parts. And the milling method can be used to investigate the cutting mechanism because the cutting force has only two components and the better chip morphology is obtained. To investigate the straight-tooth milling process of TC21 alloy, a series of milling force experiments have been done. In addition, a 3D finite element model (FEM) for the straight-tooth milling process of TC21 alloy is presented to simulate the milling process. In the model, the constitutive material model, the failure model, the friction model and the heat transfer model were adopted. Through the simulation, chip formation, stress distribution, cutting force and milling temperature were obtained. The cutting force reaches its maximum when the spindle speed reaches about 13000 rpm, and then decreases as the speed continues to increase. The results confirmed that the similar “Salomon” phenomenon existed in the cutting process of TC21 alloy.