The surface quality of parts processed by laser additive manufacturing, especially laser-based directed energy deposition (LDED), makes it difficult to meet actual use requirements. In addition, defects generated during the long-term additive manufacturing process need to be removed in time. Therefore, laser additive and subtractive manufacturing is of great significance for additive manufacturing. The main difference between laser additive-subtractive manufacturing and pure subtraction is that a cooling temperature is required due to the laser process. Therefore, this work studies the temperature variation regularity during LDED and the milling processes, as well as the surface roughness, cross-sectional microstructure, and tool wear under different cooling temperatures for milling. The results show that there is a “turning point temperature” in LDED, and the value of the turning point temperature gradually increases with heat accumulation, which affects the initial temperature of the subtractive manufacturing. When subtracting, a high initial temperature improves surface quality and reduces tool wear, but an excessively high temperature will cause the aluminum alloy to adhere to the tool. Then, the smear metal is difficult to effectively remove, deteriorates the milling quality, and aggravates tool wear. It is found that the higher the cooling temperature generated, the wider the thermally insulated shear band. The insulated shear band may affect the quality of the additive and subtractive manufacturing. Finally, it is determined that the milling temperature of aluminum alloy in this work condition is about 100 °C.