Li-rich layered oxides with high energy densities have become one kind of promising cathode for advanced lithium-ion batteries, however some issues are severely hindering their practical applications. To address these challenges, fast ion conductive LiTi2(PO4)3 (LTPO) is employed to modify the typical Li-rich cathode Li1·2Mn0·56Ni0·17Co0·07O2 (LMNCO) via a sol-gel process combined with a two-step annealing treatment in this work. Serving as a physical separator, LTPO coating effectively depresses the side reactions at cathode-electrolyte interface and the transition-metal dissolution from LMNCO active material under harsh electrochemical environment. Meanwhile, LTPO layer with high ion conductivity could facilitate the interfacial Li+ diffusion during charge/discharge process. In addition, partial Ti4+ ions doped into LMNCO effectively elevate the oxygen electronegativity and restrain the excessive oxidization of lattice oxygen, thus stabilizing the crystal structure and alleviating the stress-strain propagation upon cycling. Electrochemical characterization results demonstrate that the LTPO-modified LMNCO cathode exhibits a superior capacity retention of 86.5 % after 400 cycles at room temperature and that of 73.7 % even under an elevated temperature of 45 °C after 250 cycles under 1C. This study provides a facile strategy for the surface modification of Li-rich layered-structure oxides, which also sheds light in enhancing electrochemical performances for various cathode materials.