Currently, available gold nanoparticles (GNPs) typically accumulate in the liver and spleen, leading to concerns for their longâterm biosafety. To address this longâstanding problem, ultraminiature chainâlike gold nanoparticle clusters (GNCs) are developed. Via selfâassembly of 7â8 nm GNP monomers, GNCs provide redshifted optical absorption and scattering contrast in the nearâinfrared window. After disassembly, GNCs turn back to GNPs with a size smaller than the renal glomerular filtration size cutoff, allowing their excretion via urine. A oneâmonth longitudinal study in a rabbit eye model demonstrates that GNCs facilitate multimodal molecular imaging of choroidal neovascularization (CNV) in vivo, nonâinvasively, with excellent sensitivity and spatial resolution. GNCs targeting αvÎČ3 integrins enhance photoacoustic and optical coherence tomography (OCT) signals from CNV by 25.3âfold and 150%, respectively. With excellent biosafety and biocompatibility demonstrated, GNCs render a firstâofâitsâkind nanoplatform for biomedical imaging.