Superior　quality　of　perovskite　film　with　perfect　crystalline　and　low　defect　density　is　crucial　for　achieving　excellent　photovoltaic　performance　and　durability　of　perovskite　solar　cells　(PSCs),　and　regulation　of　growth　of　perovskite　crystal　and　defects　passivation　by　additive　is　remain　challenge.　Herein,　two　acyl　molecules　(Succinimide:　SCI,　and　Hydantoin:　HDT)　were　incorporated　into　perovskite　precursor　solution　as　additive.　It　can　be　found　that　the　HDT　molecule　can　not　only　passivate　undercoordinated　Pb2+　defects　in　perovskite　films　by　the　-C=O　groups　with　coordination　bonds,　but　also　formed　hydrogen　bonds　with　I−　by　-NH-　group,　which　effectively　inhibited　the　formation　of　iodine　vacancy　defects　and　regulated　growth　rate　of　perovskite　crystals,　and　the　quality　of　perovskite　films　was　optimized　with　enlarging　grain　size　and　reduced　trap-density.　Consequently,　power　conversion　efficiency　of　HDT-based　device　was　enhanced　from　19.47　%　to　21.00　%,　with　an　enhancement　of　JSC　and　VOC.　Moreover,　the　HDT-based　device　without　encapsulation　retained　83.7　%　of　its　initial　PCE　after　being　aged　at　10–20　%　RH　for　60　days.　Obviously,　such　a　study　could　provide　a　new　strategy　to　optimize　quality　of　perovskite　film　for　boosting　performance　of　PSCs.　©　2024　Elsevier　Ltd