The lithium residues are consumed as raw materials to in-situ synthesize the LiTiO 2 -inlaid LiNi 0.5 Co 0.2 Mn 0.3 O 2 composites. The effects of various LiTiO 2 contents on the morphology, structure, and electrochemical properties of LiNi 0.5 Co 0.2 Mn 0.3 O 2 materials are investigated in detail. Energy dispersive spectrometer mapping, high-resolution transmission electron microscopy and fast Fourier transform analysis confirm that the spherical particles of LiNi 0.5 Co 0.2 Mn 0.3 O 2 are completely coated by crystalline LiTiO 2 phase; X-ray diffraction, cross-section SEM and corresponding EDS results indicate that Ti ions are also doped into the bulk LiNi 0.5 Co 0.2 Mn 0.3 O 2 with gradient distribution. Electrochemical tests show that the LiTiO 2 -inlaid samples exhibit excellent reversible capacity, enhanced cyclability, superior lithium diffusion coefficient and rate properties. Specially, the 3mol% LiTiO 2 inlaid sample maintains 153.7mAhg −1 with 94.4% capacity retention after 100cycles between 2.7–4.4V at 1C, take 30% advantage than that of the pristine one (118.2mAhg −1 ). This improvement can be attributed to the removal of lithium residues and suitable LiTiO 2 inlaying. The absence of lithium residue is helpful to retard the decomposition of LiPF 6 . While, suitable LiTiO 2 inlaying can protect the bulk from directly contacting the electrolyte, buffer the volume change of core and shell during cycles, increase the surface electronic conductivity and offer a 3D path for Li + diffusion from the bulk to interface.