Natural materials, especially natural colorants, have achieved global prominence and might be regarded as an environmentally beneficial alternative to hazardous synthetic dyes. The color limitation of natural dyes hinders their application in textiles. The present work aims to prepare more color shades of wool yarns via dyeing with ternary natural dye mixtures without adding mordants. In this study, a sustainable dyeing approach for wool yarn was evaluated with three natural dyes, madder red (MR), gardenia blue (GB), and gardenia yellow (GY), by following an industrial dyeing procedure in the absence of a mordant. In the beginning, a preliminary assessment of dye stabilities was carried out, and it was found that the three natural dyes were sensitive to temperature and acid (degradation tendency). Then, the dyeing behavior was systematically evaluated, including a single natural dye, a binary natural dye mixture, and a ternary natural dye mixture. The results of wool yarn dyeing with a single natural dye show that the dye exhaustion percentage (E%) of MR, GY, and GB was in the ranges of 78.7–94.1%, 13.4–44.1%, and 54.8–68.5%, respectively. The dyeing results of wool yarns dyed with binary and ternary natural dye mixtures (a color triangle framework of dyed wool yarn) were characterized by colorimetric values (L*, a*, b*, C*, h, and K/S), and are presented to enlighten various colorful shades. Finally, color uniformity and colorfastness tests confirmed the vital contribution of natural dyes toward wool yarn coloration. Particularly, colorfastness to washing confirmed the stability of natural dyes with reference to the lower amount of dyes released into the effluent, which is beneficial for the environment. Overall, this study provides a good background for enhancing the industrialization trend of natural dyes by modulating their dyeing scheme.