The materials of Cyclohexylamine with 1,5-naphthalenedisulfonic acid and 3,5-dinitrosalicylic acid were used to synthesize the bis(cyclohexylammonium)-1,5-naphthalenedisulfonate (CA15NS) and bis(cyclohexylammonium)-3,5-dinitrosalicylate (CA35NS) compounds and single crystals of these compounds were grown successfully by low temperature solution growth technique. Crystal systems of the samples were identified for both the samples of CA15NS and CA35NS by the obtained unit cell parameters of the grown crystals which is determined by single crystal X-ray diffraction (SCXRD) analysis, the crystals of CA15NS and CA35NS are crystallized in monoclinic crystal structures. The powder X-ray diffraction (PXRD) analysis also was carried out for the title samples. The formations of the charge-transfer functional groups and the modes of vibrations of CA15NS and CA35NS have been confirmed by FT-IR and FT-Raman spectral analyses. The UV–Vis-NIR spectrum was carried out to find the optical behavior of the prepared crystals. The crystal of CA15NS has 232 nm and CA35NS has 207 nm as cut-off wavelength. The influences of mechanical and dielectric behavior in the crystals of CA15NS and CA35NS were investigated by means of Vickers microhardness test and dielectric study, respectively. By the thermo gravimetric analyses, the stability of the materials have been estimated for the title samples. Third order nonlinear optical study has also been studied by Z-scan technique. © 2020 Elsevier B.V.