We have designed a facile process to synthesize the hollow Fe3O4/C/CNT microspheres through a spray drying method. The composite has both the high theoretical capacity of Fe3O4 and the great electronic conductivity of carbon nanotubes (CNTs). And the hollow structure built by spray drying is beneficial to relieve the volume change during conversion reaction. With the combination of Fe3O4 and carbon materials, the Fe3O4/C/CNT microspheres show a great electrochemical performance. It has maintained a high reversible capacity of 1200mAhg(-1) after 100 cycles at the current density of 200mAg(-1) and a specific capacity of 750mAhg(-1) after 300 cycles at the current density of 1Ag(-1). The composite also shows a high initial coulombic efficiency of 75.7% at 200mAg(-1). Hence, the high-performance hollow Fe3O4/C/CNTs microsphere is a promising substitute for anode material of lithium-ion batteries (LIBs). Furthermore, the spray draying method is widely used in industrial manufacture. Therefore, this composite has greater potential for a practical application.