Lithium dendrites are easily generated for excessively-solved lithium ions (Li+) inside the lithium metal batteries, which will lead serious safety issues.In this experiment, carbon spheres (CS) are successfully anchored on TiO2(CS@TiO2) in the hydrothermal polymerization, which is filtrated on the commercial PE separator (CS@TiO2@PE). Thenegative charge in CS can suppress random diffusion of anions through electrostatic interactions. Density functional theory (DFT) calculations show that CS contributes to the desolvation of Li+, thereby increasing the migration rate of Li+. Furthermore, TiO2exhibits high affinity to liquid electrolytes and acts as a physical barrier to lithium dendrite formation. CS@TiO2 is a combination of the advantages of CS and TiO2. As results, the Li+transference number of the CS@TiO2@PE separator can be promoted to 0.63. The Li||Li cell with the CS@TiO2@PE separator exhibits a stable cycle performance for more than 600h and lower polarization voltage (17mV) at 1mA cm-2. The coulombic efficiency (CE) of the Li||Cu cells employe the CS@TiO2@PE separator is 81.63% over 130 cycles. The discharge capacity of LiFePO4||Li cells based on the CS@TiO2@PE separator is 1.73 mAh (capacity retention = 91.53% after 260 cycles). Thus, the CS@TiO2 layer inhibits lithium dendrite formation.