The　exploration　of　structural　interconversion　in　clusters　triggered　by　external　stimuli　has　attracted　significant　interest　due　to　its　potential　to　elucidate　structure-property　relationships　of　metal　clusters.　In　this　study,　two　types　of　silver　clusters,　Ag2　and　Ag6,　are　synthesized.　Interestingly,　the　clusters　exhibit　reversible　transformations　in　response　to　changes　in　the　solvent　conditions.　The　structures　and　optical　properties　of　these　clusters　are　thoroughly　characterized　using　techniques　such　as　mass　spectrometry,　single-crystal　X-ray　diffraction,　photoluminescence,　and　radioluminescence　spectroscopy.　While　both　Ag2　and　Ag6　display　excellent　photoluminescence　properties,　Ag2　demonstrates　superior　performance　in　X-ray　radioluminescence　compared　to　Ag6.　Flexible　scintillator　films　fabricated　from　Ag2　clusters　exhibit　outstanding　X-ray　imaging　capabilities,　achieving　a　spatial　resolution　of　15.0　lp/mm　and　an　impressive　detection　limit　for　an　X-ray　dose　of　0.58　μGy　s-1.　This　detection　limit　is　nearly　10　times　lower　than　the　typical　dose　rate　used　in　X-ray　diagnostics　(5.5　μGy　s-1).　This　work　introduces　a　novel　approach　for　designing　thiol-free　silver　clusters　capable　of　solvent-dependent　reversible　interconversion,　offering　new　insights　into　the　development　of　silver　clusters　for　advanced　X-ray　imaging　applications.　©　2024　American　Chemical　Society.