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PURPOSE : To improve the magneto-optical characteristics by mixing the existing fine grains having the garnet crystal structure with a specific precursor composition and baking the resultant mixture. CONSTITUTION : The crystalline grains of a high-concentration bismuth-substituted iron garnet of the formula [R is a rare earth element such as Y or La; Bi is an element substitutive with R; Fe is an element substitutive with M; M is an element such as At or Ga; R and Bi occupy each the (c) site of the garnet structure; Fe and M occupy each the (a) and/or (d) sites; O occupies the (h) site] are grown by adding aqueous ammonia to an aqueous solution of a salt containing R, a salt containing Bi, a salt containing Fe and a salt containing M so as to provide (x)<1.8 and 0<=(y)<=5, baking the resultant oxide precipitate of the respective elements, providing the existing fine grains having the garnet crystal structure, adding a suspension containing the existing fine grains to an aqueous solution containing the salt containing R, salt containing Bi, salt containing Fe and salt containing M so as to provide 1.8<=(x)<=3.0 and 0<=(y)<=5 in which the Bi is stoichiometrlcally excess, mixing aqueous ammonia therewith, affording a precipitate and baking the resultant precipitate.