Here, we report the development of a new and low-cost core-shell structure for lithium-ion battery anodes using silicon waste sludge and the Ti-ion complex. X-ray diffraction (XRD) confirmed the raw waste silicon sludge powder to be pure silicon without other metal impurities and the particle size distribution is measured to be from 200 nm to 3 μm by dynamic light scattering (DLS). As a result of pulverization by a planetary mill, the size of the single crystal according to the Scherrer formula is calculated to be 12.1 nm, but the average particle size of the agglomerate is measured to be 123.6 nm. A Si/TiO₂ core-shell structure is formed using simple Ti complex ions, and the ratio of TiO₂ peaks increased with an increase in the amount of Ti ions. Transmission electron microscopy (TEM) observations revealed that TiO₂ coating on Si nanoparticles results in a Si-TiO₂ core-shell structure. This result is expected to improve the stability and cycle of lithium-ion batteries as anodes.