Scintillators　are　the　core　components　of　real-time　dynamic　computed　tomography　(CT),　and　their　performance　directly　affects　the　radiation　dose　used　and　the　quality　of　the　output　images.　Self-trapped　exciton　scintillators　are　expected　to　resolve　the　trade-off　between　low　radiation　dose　rates　and　high　spatial　resolution.　However,　the　reported　self-trapped　exciton　scintillators　lack　systematic　design　ideas　and　the　ambiguity　of　the　emission　mechanism　limits　their　further　application　in　X-ray　imaging.　Here,　a　molecular　confinement　strategy　to　reduce　the　electronic　dimension　by　introducing　organic　molecules　with　large　ionic　radii　is　proposed　and　applied　to　design　(TPA)2Cu2I4　with　dual　self-trapped　excitons　(D-STEs).　The　D-STEs　originating　from　Jahn-Teller-like　distortion　due　to　multiple　electron-phonon　coupling　enable　(TPA)2Cu2I4　to　exhibit　a　high　PLQY　of　92　%,　a　high　light　yield　of　74,000　photons·MeV−1　and　a　low　detection　limit　of　53.1　nGyair·s−1.　In　addition,　the　(TPA)2Cu2I4　scintillation　films　also　display　excellent　imaging　quality,　with　a　spatial　resolution　of　14.1　lp·mm−1.　Impressively,　a　real-time　dynamic　X-ray　imaging　system　based　on　D-STEs　scintillators　is　established　for　the　first　time　by　coupling　with　a　thin-film　transistor　array,　verifying　its　reliability　in　nondestructive　testing　scenarios.　In　conclusion,　the　D-STEs　scintillators　created　by　molecular　confinement　have　broad　commercial　application　prospects.　©　2025