In this study, we investigated the bonding mechanism of surface-treated steel with an Al-Si alloy in order to produce steel-aluminum (STL-Al) hybrid composite materials by cast-bonding. The results showed that there are differences in the phase and properties of the hybrid composite materials bonded specimens depending on the surface treatment of the steel sheet used, and that the bonding conditions can be controlled further by detailed conditions of the surface treatment. Based on the interfacial bonding strengths measured here, the galvanized surface treatment induced metallurgical bonding to form a reaction layer on the bonding surface and was determined to be the most effective surface treatment.