We studied the melt composition to obtain pit-free, highly Bi-substituted (BiLu) 3 Fe 5 O 12 crystals by the LPE method. It was confirmed that adding B 2 O 3 to the melt increases the equilibrium segregation coefficient of Bi K 0(Bi) , and we found that a decrease in garnet composition ratio R 4 acts to increase the growth rate dependence of the normalized effective segregation coefficient of Bi K eff(Bi) / K 0(Bi) . It was also found that crystals with mirror-smooth surfaces could be obtained by adding Gd 2 O 3 to the melt. Using a melt with Gd 2 O 3 /Lu 2 O 3 ? 1, the pits which usually appear in LPE growth of (BiLu) 3 Fe 5 O 12 were eliminated, and pit-free, highly Bi-substituted (BiLuGd) 3 Fe 5 O 12 crystals were obtained. The optical properties of 250 ?m thick (BiLuGd) 3 Fe 5 O 12 crystals were measured in order to evaluate their applicability to optical isolators for use at 1.3 ?m. A sufficient Faraday rotation of ? F = ?1800 deg/cm and an extinction ratio of ?40 dB were obtained.