The spherical lithium-rich cathode material with a layered-spinel hybrid structure is successfully synthesized and coated by polyaniline (PANI). The spherical material with layered-spinel hybrid structure is firstly prepared via the hydrothermal method, and then the conducting PANI is coated on the surface of the as-prepared spherical particle through an in-situ polymerization. Based on the analysis of scanning electron microscope (SEM), transmission electron microscope (TEM), high rate transmission electron microscopy (HRTEM) and selected area electron diffraction (SAED), it can be found that the size distribution of the spherical particles modified by PANI are about ∼1 μm, meanwhile the average thickness of the PANI layer on the surface of each particle is about 6.3 nm. The electrochemical performance of the spherical lithium-rich cathode material modified by PANI is apparently improved, the capacity retention is still 92.4% after 200 cycles at a rate of 0.5 C. The discharge capacities at 0.1 C and 10 C are as high as 302.9 mAh g−1 and 146.2 mAh g−1, respectively. Therefore, the modification of PANI for the spherical lithium-rich cathode material with a layered-spinel hybrid structure will be a promising technical route for the application with high capacity, long cycle life and good safety.