Organosilicon compounds containing nitrite and oligo(ethylene oxide) substituents are synthesized as safe electrolytes for high-voltage lithium-ion batteries. We firstly report that these organosilicon electrolytes could be stably cycled at an upper cutoff voltage of 4.4 V in LiCoO2/graphite full cells. (C) 2013 Elsevier B.V. All rights reserved.