A novel composite consisted of carbon nanotubes (CNTs) and carbon-coated Li2FeSiO4 nanoparticles (Li2FeSiO4/CNTs/C) has been successfully synthesized by using spray drying technology and carbon chemical vapor deposition method. The Li2FeSiO4 nanoparticles are dispersed homogeneously in CNTs network and assembled as micro-sized porous spherical particles. Such special composite structure constructs an efficient Li+ and electron channel, which significantly enhance the Li+ diffusion coefficient and reduced the charge transfer resistance, hence may lead to exhibit high specific capacity and excellent rate performances. The Li2FeSiO4/CNTs/C composite exhibits both high initial discharge capacity and excellent cycling stability (189.2mAhg−1 at 0.1C and 71.6mAhg−1 at 5C). We believe that adding CNTs and using carbon chemical vapor deposition are effective ways to improve the electrochemical performance of Li2FeSiO4 cathode material.