The invention relates to a method for growing CaxBa1-xNb2O6 series crystals, belonging to the field of crystal growth. The method comprises the following steps: mixing powder CaCO3, BaCO3 and Nb2O5 according to the stoichiometric proportion of CaxBa1-xNb2O6, carrying out ball milling, baking, and passing through a 200-mesh screen, wherein x=0.22, 0.25, 0.28, 0.32 or 0.35; presintering, carrying out ball milling again, baking, and passing through a 80-mesh screen; putting the powder in an elongated rubber balloon, compacting, sealing, and vacuumizing to prepare a biscuit rod with uniform thickness and density under isopressing conditions; sintering the biscuit rod in a dip-coating rotary sintering furnace to obtain a compact and uniform polycrystal rod; putting the polycrystal rod in a floating region furnace, and heating at 60-100 DEG C/minute until the rod and seed crystals are molten, and abutting; and after setting the crystal growth rate at 2-5mm/hour, starting growth, and coolingto room temperature. The invention grows a CaxBa1-xNb2O6 crystal, which is 6-8mm in diameter 50-115mm long and does not have macroscopic defects, by an optical floating region process, has the advantages of high crystallization quality and high efficiency, and simplifies the technique.