The invention relates to a method for growing gallium phosphide single crystals. The method comprises the following steps of: preparing materials, charging, vacuumizing, filling gas, heating for dissolving, welding seed crystals, seeding, shouldering, removing a floating needle for the first time, removing the floating needle for the second time, performing equal-diameter control, and ending, wherein gallium phosphide polycrystals, a floating boat, a doping agent and boron oxide are put into a crucible in the material preparation process, the floating boat is made of silicon nitride and has the internal diameter of phi20 to 80mm, and pressure is controlled to be 1.0 to 5.0MPa (absolute pressure) after a hearth is filled with nitrogen. The method has the advantages that: the diameter of the crystals is controlled by the floating boat, the density of the floating boat is between the density of the boron oxide and the density of gallium phosphide, the floating boat can float on a melting surface of the gallium phosphide, and the diameter is slightly influenced by the ascending or descending of a solid liquid interface in the floating boat due to temperature change, so the diameter of the crystals can be well controlled by controlling the rotating speed of the floating boat, the gallium phosphide single crystals with the size of 1 to 3 inches are grown, the yield of the single crystals is improved, the crystallization quality of the single crystals is high, and a mobility index in electrical parameters can stably reach 130-140cm<2>/v.s.