Host-guest encapsulationo ff unctional organic dye into ap orousm etal-organic framework can give rise to the developmento fn ew functional materials. In this work, by intercalating the stilbazolium-type dye (DEAST)I (4'-diethylamino-N-methyl stilbazolium) into four lanthanide layered metal-organic complexes (Ln-LMOCs), i. e. (3), Er (4)), four responsive (DEAST)I@Ln-LMOCc omposites have been prepared, serving as multifunctional performance platform. The core-shell structures of (DEAST)I@Ln-LMOC composites have been fully characterizedb yI R, UV/Vis, PXRD, SEM, TEM, TGA and ESR. Significantly,a fter intercalation of dyes, the (DEAST)I@Ln-LMOC composites exhibit enhanced luminescent sensing properties in detecting Fe 3 + with much higherw ater stabilities. The luminescent sensing behavior stems from the fluorescencer esonance energy transfer (FRET) from the p-electron-rich BTB ligands to the Fe 3 + ,a nd their higher water stabilities are induced by electrostatici nteractions and lower porosity.S pecially,t he characteristic emissions of Sm 3 + will not be affected after the encapsulation guest dyes, which provideatheoretical guide for the modulation of luminescence devices.F inally,b etter ion conductivities andd iminished photocurrents can be achieved after the embedding of the functional organic dye. In all, the formation of (DEAST)I@Ln-LMOC composites with core-shell structures can be utilized as am ultifunctional platform with good stability.[a] L.