In this study, optimum machining parameters are evaluated for enhancing the surface roughness and hardness of AZ91 alloy using Taguchi design of experiments with Grey Relational Analysis. Dry face milling is performed using cutting conditions determined using Taguchi L9 design and Grey Relational Analysis has been used for the optimization of multiple objectives. Taguchi’s signal-to-noise ratio analysis is also performed individually for both characteristics and grey relational grade to identify the most influential machining parameter affecting them. Further, Analysis of Variance is carried to see the contribution of factors on both surface roughness and hardness. Finally, the predicted trends obtained from the signal-to-noise ratio are validated using confirmation experiments. The study showed the effectiveness of Taguchi design combined with Grey Relational Analysis for the multi-objective problems such as surface characteristics studies.