Highly directional white-light generation was recently reported for the organotin sulfide cluster [(StySn)(4)S-6] (Sty = p-styryl). This effect was tentatively attributed to the amorphous nature of the material in combination with the specific combination of an inversion symmetry-free T/E cluster core (T = tetrel, E = chalcogen) with the attachment of ligands that allow pi delocalization of the electron density. Systematic variation of T and the organic ligand (R) that runs from T = Si through Ge to Sn and from R = methyl through phenyl and p-styryl to 1-naphthyl provides a more comprehensive view. According to powder X-ray data, only [(PhSi)(4)S-6] is single-crystalline among the named combinations. Here we demonstrate the fine-tuneability of the nonlinear response, i.e., changing from white-light generation to second harmonic generation as well as controlling the white light properties. These are investigated as a function of T, delocalization of the electron density within R, and the order within the molecular solids.