Perovskite　nanocrystals　(PNCs)　have　attracted　widespread　attention　as　promising　materials　for　the　optoelectronic　field　due　to　their　remarkable　photophysical　properties　and　structural　tunability.　However,　their　poor　stability　and　the　use　of　toxic　organic　solvents　in　the　preparation　process　have　severely　restricted　their　practical　applications.　Herein,　a　facile,　rapid　and　toxic　organic　solvent-free　synthesis　strategy　of　CsPbBr3　PNCs　was　developed　for　the　first　time　via　the　ligand-assisted　reprecipitation　(LARP)　method　using　natural　deep　eutectic　solvents　(NADESs)　as　solvents　and　surface　ligands.　In　this　method,　the　NADESs　not　only　functioned　as　solvents　for　green　synthesis,　but　also　served　simultaneously　as　surface　ligands　of　CsPbBr3　PNCs　to　significantly　improve　their　optical　properties　and　stability.　The　as-synthesized　CsPbBr3　PNCs　exhibited　high　photoluminescence　quantum　yield　(PLQY,　∼96.8%),　narrow　full　width　at　half-maximum　(FWHM,　∼18.8　nm)　and　a　high　stability　that　retained　82.9%　of　PL　intensity　after　70　days.　This　work　provides　a　new　strategy　for　the　green　synthesis　of　PNCs,　which　promises　feasibility　for　the　industrial　large-scale　synthesis　of　high-quality　PNCs.　©　2022　The　Royal　Society　of　Chemistry.