Chip morphology and its formation mechanisms, cutting force, cutting power, specific cutting energy, tool wear, and tool wear mechanisms at different cutting speeds of 100–3000 m/min during dry face milling of Ti-6Al-4V alloy using physical vapor deposition-(Ti,Al)N-TiN-coated cemented carbide tools were investigated. The cutting speed was linked to the chip formation process and tool failure mechanisms of the coated cemented cutting tools. Results revealed that the machined chips exhibited clear saw-tooth profile and were almost segmented at high cutting speeds, and apparent degree of saw-tooth chip morphology occurred as cutting speed increased. Abrasion in the flank face, the adhered chips on the wear surface, and even melt chips were the most typical wear forms. Complex and synergistic interactions among abrasive wear, coating delamination, adhesive wear, oxidation wear, and thermal mechanical–mechanical impacts were the main wear or failure mechanisms. As the cutting speed was very high (>2000 m/min), discontinuous or fragment chips and even melt chips were produced, but few chips can be collected because the chips easily burned under the extremely high cutting temperature. Large area flaking, extreme abrasion, and serious adhesion dominated the wear patterns, and the tool wear mechanisms were the interaction of thermal wear and mechanical wear or failure under the ultra-high frequency and strong impact thermo-mechanical loads.