It is important for the further improvement of lithium-ion battery energy densities to develop high-specific-capacity cathode materials. Li3V2O5 has attracted much attention due to its high specific capacity, even exceeding 240 mA?偸h/g. However, its low electrochemical cycling stability induced by the low Li+ transport dynamics and irreversible phase transition restricts the application of Li3V2O5 cathode materials in lithium-ion batteries. In this paper, co-doped Li3V2O5 nanorod cathode materials were prepared. The one-dimensional structure can relieve the accumulation of strain during charging and discharging process. Also, Co3+ doping can stabilize the structure of Li3V2O5 by forming the more intense Co-O bonds. Furthermore, Co3+ doping expands the cell volume and ratio of V4+ in Li3V2O5. These collectively result in the improved Li+ diffusion coefficient and cycling stability of Li3V2O5. The 1% Co-doped Li3V2O5 (i.e., 1%Co-LVO sample) has a specific discharge capacity of 256.43 mA?偸h/g at a current density of 50 mA/g and a capacity retention rate of 77.3% after 100 cycles, which is 28% greater than that of the pristine Li3V2O5. 1%Co-LVO sample shows a superior capacity fading (i.e., 0.23%/cycle). This paper can provide an effective method for the preparation and performance regulation of high-energy-density lithium-ion cathode material (i.e., Li3V2O5).