Surface coating approaches for silicon (Si) have demonstrated potential for use as anodes in lithium-ion batteries (LIBs) to address the large volume change and low conductivity of Si. However, the practical application of these approaches remains a challenge because they do not effectively accommodate the pulverization of Si during cycling or require complex processes. Herein, Si-embedded titanium oxynitride (Si-TiON) was proposed and successfully fabricated using a spray-drying process. TiON can be uniformly coated on the Si surface via self-assembly, which can enhance the Si utilization and electrode stability. This is because TiON exhibits high mechanical strength and electrical conductivity, allowing it to act as a rigid and electrically conductive matrix. As a result, the Si-TiON electrodes delivered an initial reversible capacity of 1663 mA h g−1 with remarkably enhanced capacity retention and rate performance.