Bis(cyclohexylammonium) terephthalate (BCT) and cyclohexylammonium 4-methoxy benzoate (C4MB) single crystals were successfully grown by the slow evaporation solution growth technique. The harvested crystals were subjected to single-crystal X-ray diffraction, spectral, optical, thermal and mechanical studies in order to evaluate physiochemical properties. The Kurtz and Perry technique for second harmonic generation (SHG) study revealed that the powdered materials of BCT and C4MB exhibit SHG efficiency 0.2 times less and 1.3 times greater than that of standard reference material potassium dihydrogen phosphate. C4MB crystal exhibits high efficiency than BCT, because of methoxy group substituted in the para position of phenyl ring. With high SHG efficiency and thermal stability para substituted C4MB crystal will be a potential candidate for optical device fabrication.