The growth technique and physical properties of SiGe multicrystals with microscopic compositional distribution are demonstrated for new high-efficiency solar cells in which the wavelength dependence of the absorption coefficient can be freely designed by controlling the compositional distribution in the SiGe multicrystals. This growth technique is suitable for the practical casting method, and it is made up of melt growth of SiGe multicrystals with wide and microscopic distribution of the composition from Si to Ge all over the crystals. It is studied how much widely the microscopic compositional distribution in SiGe multicrystals grown from binary Si-Ge melts can be controlled by the melt composition and the cooling process. The range of the microscopic compositional distribution becomes wider as the starting Si concentration in the growth melt becomes larger. SiGe multicrystals with various microscopic compositional distribution can be freely controlled by optimizing the melt composition and the cooling process. The wavelength dependence of the absorption coefficient of such SiGe multicrystals can be also freely designed. These results show that SiGe multicrystals with microscopic compositional distribution are hopeful for new high-efficiency solar cell applications by using the practical casting method.