Zeolitic materials are commonly used to capture emergent contaminants in water or complex aqueous effluents. The efficiency of this adsorption depends strongly on the guest–host interactions and on the surrounding environment with possible coadsorption of the solvent. Only a few experimental techniques are available to probe in situ the sequestration processes at the solid/liquid interface. We propose in the present work to combine the second harmonic scattering technique with isothermal titration calorimetry in order to investigate the adsorption and the confinement of a hemicyanine dye adsorbed inside faujasite materials. The methodology described here permits the quantification of the correlations between the confined dyes in the material and thus gives local information about the organization at the nanometer scale. Various impacts, such as the effect of the solvent type and the silicon to aluminum ratio of the zeolitic adsorbent, are quantitatively estimated and discussed. This work highlights that the most correlated system matches the higher adsorption capacity associated with the lower entropic contribution.