We have discussed in detail the optimum pre-mordanting conditions of vanadium in the dyeing of wool with sumac gallnut as a natural plant dye. The optimum conditions of pre-mordanting were 5 mM of vanadium at 100 °C and 50 % owf of sumac gallnut. After mordanting, vanadium was distributed over the wool epidermis. The resultant vanadium black complex plays an important role in developing the colored products, with sumac gallnut having a low affinity for wool. To develop the dyeing method with excellent utility, we compared the toxicities of vanadyl sulfate with those of copper sulfate to Oryzias latipes. We showed that vanadyl sulfate is less toxic than copper sulfate. Moreover, experimental calculations of vanadium concentration showed that the low concentration of vanadium used in the present study has toxicity similar to that found in nature. © 2014 Jpn. Res. Assn. Text. End-Uses.