The　simultaneous　achievements　of　lower　aspect　ratio　and　larger　crystal　size　is　urgent　for　the　production　of　high-quality　sucralose.　In　this　work,　non-toxic　ethanol-based　anti-solvent　crystallization　(ASC)　of　sucralose　was　conducted,　during　which　carboxylic　acids　bearing　different　alkyl　lengths　(isovaleric　acid　(IVA),　hexanoic　acid　(HNA),　octanoic　acid　(ONA),　decanoic　acid　(DNA))　were　used　as　anti-solvents.　The　longer　alkyl　lengths　of　carboxylic　acids　can　render　higher　sucralose　yield　because　the　better　flexibility　can　provide　larger　free　void　spaces　with　facilitation　of　emulsion　shrinking,　resulting　in　higher　crystallization　ratio　and　rate.　Also,　the　ASC　conditions　have　been　optimized,　based　on　which　low　aspect　ratio　(1.5585)　and　small　particle　size　(15.755　mu　m)　can　be　obtained　using　ONA　as　an　anti-solvent.　Based　on　single-crystal　structure　analysis,　the　ONA-treated　product　bearing　relatively　weaker　O-H　&　ctdot;O/C-H　&　ctdot;Cl　hydrogen　bonds　was　adopted　for　further　ultrasound-assisted　ASC　process.　Interestingly,　upon　the　intermittent　sonication　mode,　the　sucralose　product　with　ultra-low　aspect　ratio　(1.244)　and　larger　crystal　size　(42.722　mu　m)　can　be　obtained,　which　is　attributed　to　the　relatively　stronger　sp3-C-H　&　ctdot;Cl0　hydrogen　bonds　on　the　{011}　face　than　O-H　&　ctdot;O　bonds　on　the　{101}/{110}　faces.　This　work　will　provide　a　theoretical　guide　for　the　production　of　high-quality　sucralose.