Nonlinear optical crystals plays important role in the field of photo electronics, optical communication, optical modulators, laser spectroscopy, frequency conversion and so on. Semi-organic crystals exhibit high NLO response, thermal stability, laser damage threshold, mechanical stability, wide optical window transmittance and structural diversity. Combinations of inorganic and organic molecules yield the semi-organic crystals. Based on its structural diversity it’s classified into three categories. In this chapter explains various kinds of semi-organic crystals and their optical, thermal, mechanical, laser damage threshold value and NLO properties and also explains the importance of these crystals in the field of optoelectronics, frequency conversion and other optical applications.