The electrode surfaces of degraded lithium-ion batteries (LIB) were analyzed by liquid chromatography-quadrupole time of flight mass spectrometry (LC-QTOF/MS). The solid-electrolyte interphase (SET) layer influences the performance of LIBs. Therefore, we conducted a study aimed at clarifying the deterioration mechanism of LIBs by examining the components in the SET before and after degradation due to cycling. We believe that the change in the mass transfer characteristics at the electrode interface influenced by SET deterioration can be clarified via Lc-QTOF/MS, which would allow elucidation of the deterioration mechanism. The analysis results showed that the degradation products contain multiple components, including polymers of carbonate compounds and phosphate esters, which are formed via electrochemical and chemical reactions, resulting in remarkably reduced capacity. The results suggest that LC-QTOF/MS is a valuable technique for the degradation analysis of LIBs. (C) The Author(s) 2015. Published by ECS. All rights reserved.