Vanadium　sulfide　was　first　employed　as　a　cathode　for　all-solid-state　lithium-ion　batteries　and　demonstrated　superior　compatibility　with　the　solid　electrolyte,　in　which　the　interface　between　the　electrode　and　solid　electrolyte　has　been　optimized.　Consequently,　it　can　exhibit　excellent　electrochemical　performance　in　the　voltage　range　of　1.5–3.5　V.　Moreover,　the　ex-situ　X-ray　photoelectron　spectroscopy　measurements　reveal　the　incomplete　conversion　mechanism　to　account　for　the　superior　electrochemical　performance.　Specifically,　the　electrode　of　VS2　exhibits　a　large　capacity　of　268.1　mA　h　g−1　at　50　mA　g−1　(rate　performance).　At　a　current　density　of　100　mA　g−1,　a　large　reversible　capacity　of　215　mA　h　g−1　can　be　maintained　after　100　cycles,　indicating　extraordinary　cycling　stability,　making　it　a　promising　electrode　for　high　energy　density　all-solid-state　lithium-ion　batteries.　©　2022,　Science　China　Press　and　Springer-Verlag　GmbH　Germany,　part　of　Springer　Nature.