Large sized α-Li 3 Fe 2 (PO 4 ) 3 single crystals with high quality are successfully grown by a flux method. Magnetic behaviors of the grown crystals are investigated by means of magnetic susceptibility, magnetization, and heat capacity measurements along different directions. The results confirm that α-Li 3 Fe 2 (PO 4 ) 3 exhibits weak ferrimagnetic behaviors at low temperature, which are in good agreement with those reported previously. However magnetic anisotropy is confirmed for the first time, suggesting that the c-axis is the likely magnetic easy axis and the a-axis is the magnetic hard one. Two anomalies are clearly observed in magnetic susceptibility along the a-axis and heat capacity data at zero field, suggesting the appearance of two successive magnetic transitions at ~26 and ~22K in the system.