The molecular interactions of MC-540 (Merocyanine 540) in clay suspensions containing natural bentonite and CTAB (cetyl trimethyl ammonium bromide)-modified bentonite were examined by using absorption, steady-state and time-resolved fluorescence spectroscopies. Strong affinity of clays for dye adsorption caused the strong interaction of MC-540 molecules with bentonite particles in aqueous dispersion. The interaction of dye with natural bentonite and CTAB-modified bentonite particles in aqueous dispersion caused significant changes in the photophysical properties of MC-540 when they were compared to those in pure water. Spectral data revealed that monomer, H-dimer and H-aggregate of MC-540 in the clay aqueous dispersions were formed depending on dye concentration. Moreover, H-aggregates of dye were predominantly formed in the CTAB-modified bentonite aqueous suspension. The presence of H-aggregates strongly decreased the fluorescence lifetime of MC-540. (C) 2014 Elsevier B.V. All rights reserved.