Organosilicon compounds have attracted considerable interest as electrolytes for lithium-ion batteries because they are nontoxic, nonflammable, as well as have lower glass transition temperatures, lower vapor pressure and higher flash point than commerical alkyl carbonates. These compounds can improve the electrochemical performances and safety of lithium-ion batteries when used as electrolyte solvents or additives in the electrolytes. In this paper, the recent advances of organosilicon compounds both as electrolyte solvents and additives are reviewed. Organosilicon electrolytes containing ethylene oxide (EO) substituents with or without carbon spacer between silicon atom and EO unit are specially remarked as safe electrolytes. Organosilicon compounds as functional additives are also introduced in terms of the capabilities of passive film formation, flame-retardant, and acid/water scavenger.