Although　sodium-based　conversion　materials　are　promising　as　anodes　for　sodium-ion　batteries,　with　evident　superiority　in　terms　of　storage　capacity,　continuous　performance　deterioration　occurs　due　to　the　structural　degradation　during　cycling.　Herein,　by　substituting　the　SbPS4　matrix　with　different　amounts　of　Se,　the　targeted　compounds　with　multiple　stoichiometries,　including　SbPS3Se,　SbPS2Se2,　and　SbPSSe3　are　prepared.　Introducing　the　guest　element　of　Se　into　the　parent　thiophosphate　can　effectively　retain　the　advantage　of　the　thiophosphate,　and　replacing　S　with　Se　is　beneficial　to　the　modulation　of　electronic　structure,　the　expansion　of　lattice　spacing,　and　the　enhancement　of　electrochemical　performance.　As　a　result,　the　optimized　SbPS3Se　material　exhibits　the　highest　reversible　capacity　(740.12 mA　h　g−1　at　a　current　density　of　0.1 A　g−1)　and　excellent　cycling　performance　(over　69%　capacity　retention　after　100　cycles).　However,　with　a　further　increase　in　Se　substitution　content,　the　stability　of　the　structure　decreases　because　the　diameter　of　thiophosphate　nanotube　materials　increases　continuously,　leading　to　inferior　electrochemical　properties.　Therefore,　moderate　Se　substitution　is　beneficial　to　the　improvement　of　the　electrochemical　performance　of　SbPS4　materials.　The　Se　substitution　strategy　can　provide　an　important　reference　value　for　the　design　and　optimization　of　conversion　anode　materials.　Graphic　Abstract:　[Figure　not　available:　see　fulltext.]　©　2022,　The　Minerals,　Metals　&　Materials　Society.