Titanium matrix composite (TiB+TiC)/TC4 has excellent physical properties and is a completely new composite material with great application prospects in the next generation of the aerospace field. However, there are problems, such as tool loss and material overheating, when using conventional processing methods. Electrochemical milling is a low-cost, high-efficiency processing method for difficult-to-machine metal materials with no tool wear. In this research, the feasibility of the electrochemical milling of (TiB+TiC)/TC4 and removal mechanisms during processing was reported for the first time. The feasibility of electrochemical milling is verified by the current efficiency experiment and basic processing experiment. Through the adjustment of the processing parameters, the final material removal rate increased by 52.5% compared to that obtained in the first processing, while the surface roughness decreased by 27.3%. The removal mechanism during processing was further performed based on the current efficiency experiment; three stages were observed and concluded during the electrolytic dissolution. This research proved that electrochemical milling is an excellent low-cost method for roughing and semi-finishing (TiB+TiC)/TC4 composites and provides guidance for better electrochemical milling in the titanium matrix composites.