A series of new organic dye-interleaved nanocomposites (NCs) were prepared by intercalation of alizarin-3-sulfonate anion (Az3S) into Zn-Al-layered double hydroxide (LDH) inorganic lamella host at different concentrations via self-assembly method. The physicochemical properties of the as-synthesized LDH and NCs were studied using PXRD, FTIR, ICP-AES, CHNS, true density and SEM techniques. Basal spacing expansions from 9.0 Å in LDH to about 10.0 and 20.0 Å in the resulting NCs were observed, suggesting that Az3S was probably orientating itself in two or more different ways in the host-matrix due to two different species that co-existed in the mother liquor during the synthesis. FTIR study on NCs further confirmed the interleaving by showing combined patterns of LDH and Az3S. Changes in chemical composition in NC, particularly the increase in carbon and sulfur content compared to the LDH were in strong agreement with the PXRD and FTIR studies. In addition, the inclusion of an organic moiety as interleaving guest in NCs was found to reduce the true density and significantly alter the microscopic surface morphology of the resulting NCs.