Gold　nanoclusters　(AuNCs)　are　emerging　as　promising　functional　probes　for　bioapplications.　However,　because　of　rapid　renal　clearance,　it　is　a　challenge　to　tailor　their　biofate　and　improve　their　disease-targeting　ability　in　vivo.　Herein,　we　report　an　efficient　strategy　to　tailor　their　organotropic　actions　by　rationally　designing　AuNC　assemblies.　The　nanocluster　assembly　is　established　based　on　the　moderate　electrostatic　interaction　or　strong　coordination　between　AuNCs,　enabled　by　solely　chitosan　(CS)　or　the　coadded　chelating　metal　ions　(e.g.,　Gd3+).　We　show　that　AuNCs-CS　is　rapidly　excreted　into　urine,　while　further　coordination　of　Gd3+　confers　assemblies　with　liver　and　lung　accumulation　capabilities,　dependent　on　Gd3+　contents.　The　organotropic　actions　are　unraveled　to　result　from　their　tunable　stability　in　vivo　and　binding　capability　to　cells/proteins.　We　also　demonstrate　that　lung-targeting　assemblies　can　enable　specific　NIR-II　luminescence　imaging　of　lung　orthotopic　tumors,　which　cannot　be　realized　by　employing　discrete　AuNCs.　We　anticipate　that　these　findings　will　offer　insights　into　the　design　principles　of　metal　nanocluster　probes　and　related　bioapplications.　©　2024　American　Chemical　Society.