Hybrid　perovskite　solar　cells　(PSCs)　have　emerged　as　a　promising　alternative　to　crystalline　silicon　solar　cells,　owing　to　their　excellent　photovoltaic　characteristics　and　straightforward　fabrication　processes.　However,　the　rapid　crystallization　dynamics　frequently　results　in　unfavorable　film　morphology,　giving　rise　to　a　plethora　of　defect　sites　and　fostering　the　formation　of　trapped　non-radiative　recombination　centers,　thus　limiting　the　further　advancement　and　refinement　of　PSC　technology.　In　this　study,　we　introduce　N-benzoylthiourea　(N-BzTu)　molecules　as　a　passivate　agent　within　PSCs　through　anti-solvent　additive　approach.　The　incorporation　of　[sbnd]C[dbnd]O　and　[sbnd]C[dbnd]S　functional　groups　in　N-BzTu　effectively　passivates　the　under-coordinated　Pb2+　defects,　while　the　formation　of　robust　hydrogen　bonding　interactions　between　[sbnd]NH[sbnd]　or　[sbnd]NH2　groups　and　I−　ions　acts　as　a　potent　inhibitor　against　the　generation　of　iodine　vacancy　defects.　This　dual-action　mechanism　not　only　addresses　the　issue　of　defect　proliferation　but　also　enhances　the　overall　structural　integrity　of　the　PSC　film.　Moreover,　by　meticulously　adjusting　the　growth　rate　of　the　perovskite　crystals,　we　can　achieve　dense　and　uniformly　distributed　perovskite　films.　Specifically,　the　power　conversion　efficiency　(PCE)　of　the　optimized　devices　soared　from　22.11　%　to　an　impressive　24.05　%.　Consequently,　the　hydrothermal　stability　of　the　device　is　also　improved,　with　the　initial　efficiency　of　the　unencapsulated　device　remaining　above　80　%　after　1540　h　at　20–25　%　relative　humidity.　©　2025　Elsevier　Inc.