Aspirin (abbr. ASA) is intercalated into the layered terbium hydroxide (LTbH) by anion exchange method. Structure, chemical compositions, thermostability, morphology, luminescence property, cytotoxic effects and controlled-release behaviors have been investigated. The ASA molecules may embed between layers with monolayered vertical arrangement, and the thermal stability of organics was enhanced after intercalation. The Tb 3+ luminescence in ASA-LTbH composites was enhanced compared with LTbH precusor and the luminescence intensity increased with the deprotonation degree. The cytotoxic effect of LTbH was observed with a sulforhodamine B (SRB) colorimetric assay, which revealed that the LTbH showed low cytotoxic effects. In addition, the ASA-LTbH composites exhibited a sustained release of ASA in Na 2 HPO 4 -NaH 2 PO 4 buffer solution at pH 6.86 and 37°C. Construction of LRHs composites with drug molecules provided a beneficial pathway for preparing biohybrid based on LRHs, which may have potential applications in drug delivery carrier and biological fluorescence probe.