Oriented polycrystalline rods of Tb 0.36 Dy 0.64 (Fe 1− x Co x ) 2 (where x = 0.00, 0.10, 0.15, 0.20, 0.30) have been successfully prepared by zone melting unidirectional solidification with high growth velocity of 240mm/h and 900mm/h. The measurement results show that 〈110〉 preferred orientation can be formed in the quaternary alloys with dendritic solidified morphologies. The magnetostriction was measured as a function of applied magnetic field up to 4kOe and compressive stresses of 5MPa and 10MPa over a wide temperature range from −80 to 100°C. The magnetostriction “jump” effect was obvious in all the Tb 0.36 Dy 0.64 (Fe 1− x Co x ) 2 〈110〉 oriented crystals at room temperature and elevated temperature (100°C), but not so obvious at cryogenic temperature (−80°C). A satisfactory magnetostrictive property was obtained in the 〈110〉 oriented Tb 0.36 Dy 0.64 (Fe 0.85 Co 0.15 ) 2 crystal with the value of 1810 × 10 −6 under 14MPa pre-stress and 5kOe magnetic field at room temperature.