Cross-linkable polysiloxane-epoxides were synthesized and investigated as new electrode binders for lithium-ion batteries. Mesocarbon microbead (MCMB) electrodes were prepared with a series of polysiloxane-epoxides precursors thermally cross-linked by polyamines and evaluated electrochemically in MCMB/Li cells. We demonstrated that the composition and functionality of the new cross-linked binders play a significant role in the lithium-ion cell performance (C) 2013 The Electrochemical Society. All rights reserved.