The present disclosure relates to a method for making an electrode material of lithium-ion batteries. In the method, a lithium source solution and a plurality of titanium source particles are provided. The lithium source solution and the titanium source particles are mixed, wherein a molar ratio of lithium element to titanium element is in a range from about 4:5 to about 9:10, thereby forming a sol. A carbon source compound is dispersed into the sol to form a sol mixture. The sol mixture is spray dried to form a plurality of precursor particles. The precursor particles are heated to form a lithium titanate composite electrode material.