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The spherical Li4Ti5O12 used in lithium-ion-batteries was synthesized by a spray-dryer method, and the influence of the doping of carbon and Mg2+ to the material was studied.The materials were characterized in structure、 morphology and performance by means of XRD, SEM, BET, Laser Particle diameter and electrochemical tests.Results show that the Li4Ti5O12 materials prepared by this method are spherical, the tap-density is as high as 1.60g/cm3, initial reversible specific capacity is 163.8 mAh·g-1.Furthermore, the high rate discharge capacity of the material was significantly improved by C and Mg2+ additive, When the spherical Li4Ti5O12/C composite synthesized by the emulsion-sprayed method used in full cell the retention rate of capacity was 94.5% after the 300th cycle, and the charge capacity at the rate of 10C is 91.2% of that at 1C, the discharge capacity at the rate of 15C is 90.2% of that at 1C.The high value of application of this spherical Li4Ti5CO12/C composite was displayed when used as cathode material in batteries of HEV.