Inspired by the iron gall ink that has been used since the Middle Ages, we formulated a hair-dyeing solution for blackening hair. The ingredients in the formulation have been approved as cosmetic ingredients, including tannic acid, gallic acid, and Fe(d-gluconate)₂. The formulation does not require any harmful oxidizing agents, such as hydrogen peroxide—the Fe(II) cations bound to tannins are oxidized spontaneously upon exposure to air and form the blackish Fe(III)-tannin nanocomplex that coats hair firmly. In our study, we show that the dyed color did not fade under sunlight exposure for at least three months and after shampooing. This natural formulation for black hair-dyeing can have great impact in the hair cosmetic industry.