A pyrazino-1,3a,6a-triazapentalene dye-based molecule was intercalated by direct co-precipitation method into the galleries of negatively charged layered double hydroxide (LDH) to form a new luminescent LDH filler. The materials of cation composition Zn/Al = 2 lead to well-defined organic inorganic assemblies. The structure of the hybrid materials was characterized by X-ray diffraction (XRD), Fourier-transform infrared spectra (FTIR) and UV–visible spectra. Optical properties of the materials, at both solid state and slurry state, were also recorded and absolute photoluminescent quantum yields (PLQY) were determined showing that the nanohybrid LDH slurry exhibited higher luminescence properties under UV excitation than the corresponding LDH powder. LDH fillers were used to prepare composite films by dispersion in both hydrophobic or hydrophilic polymer matrix such as poly (dimethyl siloxane) (PDMS) and poly(ethylene oxide) (PEO), respectively. Composite films were characterized by Small Angle X-ray Scattering (SAXS) and PLQY were recorded in order to compare the behaviour of the nanohybrid LDH filler in both polymer matrices. It was found that the aggregation of particles is still observed by SAXS.