Four phenyl-substituted quinolinium salts with different counter anions, C27H27NO4S, C26H25NO5S, C25H22NO5SCl, and C25H22NO5SBr, were synthesized and their single crystals were successfully grown from methanol solution by slow evaporation. Single crystal X-ray diffraction analyses showed that C27H27NO4S crystal belongs to the noncentrosymmetric orthorhombic space group Pna2(1), and the other three crystals belong to centrosymmetric monoclinic space group P2(1)/n. Their first order hyperpolarization and macroscopic nonlinearity were analyzed and physical properties were characterized by UV-vis absorption spectroscopy, and differential scanning calorimetric and thermal gravimetric analysis. (C) 2015 Elsevier B.V. All rights reserved.