TiAlN-coated carbide tools have been used to machine Ti-6Al-4V alloys in aviation workshops. However, the effect of TiAlN coating on surface morphology and tool wear in the processing of Ti-6Al-4V alloys under various cooling conditions has not been reported in the public published literature. In our current research, turning experiments of Ti-6Al-4V with uncoated and TiAlN tools under dry, MQL, flood cooling, and cryogenic spray jet cooling conditions were carried out. The machined surface roughness and tool life were selected as the two main quantitative indexes for estimating the effects of TiAlN coating on the cutting performance of Ti-6Al-4V under various cooling conditions. The results showed that TiAlN coating makes it hard to improve the machined surface roughness and tool wear of a cutting titanium alloy at a low speed of 75 m/min compared to that achieved by uncoated tools. The TiAlN tools presented excellent tool life in turning Ti-6Al-4V at a high speed of 150 m/min compared to that achieved by uncoated tools. From the perspective of obtaining finished surface roughness and superior tool life in high-speed turning Ti-6Al-4V, the selection of TiAlN tools is feasible and reasonable under the cryogenic spray jet cooling condition. The dedicative results and conclusions of this research could guide the optimized selection of cutting tools in machining Ti-6Al-4V for the aviation industry.