Gd2PdSi3single crystals were grown by a vertical floating zone method with radiation heating at a zone traveling rate of 3 mm/h. The compound exhibited congruent melting behavior at a liquidus temperature of about 1700 °C. The slightly Pd-depleted composition of the crystal, with respect to the nominal Gd2PdSi3stoichiometry, led to gradual accumulation of Pd in the traveling zone and to a decreasing operating temperature during the growth process. Thin platelet-like precipitates of a GdSi phase were detected in the stoichiometric feed rod growth crystal matrix which can be reduced by annealing treatment. Feed rod composition shift crystal growth was proved to be a better way of getting high quality of Gd2PdSi3single crystal.