The sensitization properties of two squaraine dyes adsorbed onto the van der Waals surface of n-doped tin disulfide single crystals were studied using atomic force microscopy (AFM), vis-NIR absorption spectroscopy, and photoelectrochemical techniques. Quantum yield per absorbed photon (QYAP) values of near unity were observed for submonolayer coverages of 2,4-bis(4-(N-methyl-N-hexylamino)phenyl)squaraine (1-6SQ) in aqueous electrolyte when a sufficiently positive bias was applied, demonstrating the advantages of SnS2 as a photoanode for fundamental studies of dye sensitization. Islandlike and microcrystalline morphologies, associated with aggregate formation and revealed by AFM, could be correlated with spectral shifts in both the absorbance and photoaction spectra. A related dye, 2,4-bis(4-N, N-dimethyl)-2-hydroxyphenyl)squaraine (1-1OHSQ), at similar coverages showed slightly lower QYAP, ascribed to a recombination path due to the different aggregate structures.