SrO⋅(6-x)Fe2O3⋅xAl2O3 solid solution crystals were grown from two series of melts of compositions expressed as 0.85(SrO⋅B2O3)-0.15 [SrO⋅(6-y1)Fe2O3⋅y1Al2O3] and 0.875(1.5SrO⋅B2O3)-0.125[SrO⋅(6-y2)Fe2O3⋅y2Al2O3], where 0<y1, y2y2 series with y2 value more than 4.5. From the melt of y1 series, the solid solution crystals could be obtaind for all y1 values. The concentration ratio of aluminium to iron of the crystals grown from a melt of y2 series was considerably smaller than the same concentration ratio in the melt from which the crystals was grown. Crystals with the x values of 0.82, 1.51, 3.54, 5.25 were obtained from the melts with the y1 value 2, 3, 4, 5, respectively. These results suggest that the molar ratio SrO/Al2O3 of melts should be less than 1.5 to get crystals with high Al content. Most of the crystals were hexagonal thin plate with 1cm-0.1mm across. The higher the Al content in the crystals, the smaller the crystal size. Other crystalline phase did not precipitate for all composition and temperature range in the present experiment. Lattice parameter and Curie temperature were also measured for the solid solution crystals.