Aluminum alloy is widely used in many products because of its high strength, lightweight, good formability, and other excellent properties. When using aluminum alloy in lightweight structures, mechanical properties such as hardness, strength, and elongation are considered. However, mechanical properties are subject to the impact of a variety of controllable factors including heat treatment, which leads to quality instability. This study applied A6066 aluminum alloy for age hardening with solution temperature, quenching temperature, artificial aging temperature, and artificial aging time using the T6 heat treatment for controlling these factors. This study adopted the Taguchi Method to design the experiments, and integrated with Grey Relational Analysis to discuss problems associated with multiple quality characteristics, in order to determine the overall optimal combination of manufacturing process parameters. This study was validated by actual experiments, and the expected results improved the mechanical properties of aluminum alloy. Research findings suggested that the optimal combination of manufacturing process parameters issolution temperature at 530 °C, quenching at room temperature, artificial aging temperature at 190 °C, and artificial aging time at 4 hours. The ANOVA (analysis of variance) indicated that the artificial aging temperature was the most important factor affecting the multiple quality characteristics. Finally, the comparison of the experimental results with the data of the experimental group of highest Grey Relational Grade indicated that the alloy hardness improved by 3.38%, the tensile strength in the vertical direction (T) improved by 8.79%, and the tensile strength in the parallel direction (L) improved by 10.73%.