Anatase TiO2 nano-particles anchored on layered cathode material of Li[Li0.2Ni0.13Co0.13Mn0.54]O2 has been prepared for the first time through the co-precipitation method. The structure and electrochemical performance of this modified layered cathode material are systematically investigated. XRD and SEM indicate that these TiO2 NPs-anchored electrodes have good layered structure and regular morphology, respectively. XPS, AFM and TEM have proved that the TiO2 nanoparticles (NPs) are anchored on the surface of the particles and distributed uniformly. Compared with the bare electrode with initial discharge capacity of 248.0mAhg−1 and capacity retention of 66.65% after 100 cycles at 0.5C, 0.5% TiO2 NPs-anchored electrode exhibits a capacity of 243.8mAhg−1 with capacity retention of 84.40% by electrochemical tests. Furthermore, the 0.5% TiO2 NPs-anchored electrode could deliver the initial discharge capacity of 265.9mAhg−1, 243.8mAhg−1, 190.8mAhg−1, 134.3mAhg−1 corresponding to 0.2C, 0.5C, 2C and 5C, respectively. The anchored TiO2 NPs could effectively reduce the interfacial resistance between the cathode and the electrolyte and benefit the Li+ conduction in the electrode compared with the traditional coated layers. Anchoring TiO2 NPs on the surface of electrode is firstly adopted to enhance the electrochemical properties of layered cathode materials for lithium-ion batteries.