Solid-state CPL measurements were performed for the first time on hybrid, laminar materials based on γ-ZrP pillared with organic diphosphonates. Ad hoc optically pure diphosphonates were synthesized and the luminescence properties of their complexation with Tb(III) were verified in solution. CD and CPL measurements showed that the bistriazolylpyridine chromophores bonded to the metal provided an effective chiral environment that produced significant signals. In the case of the γ-ZrP-derived materials, experimental evidence and simple molecular modeling hinted to the occurrence of supramolecular chirality in the particles, induced by the intrinsic dissymmetry of the organic diphosphonates or by the intercalation of chiral species such as 1-phenethylamine. Chirality at the supramolecular level was revealed in the solid state by the CPL signals measured from reporter Tb(III) ions intercalated in the hybrid matrix.