The advent of high intensity lasers coupled with the recent advances in crystal technology has led to rapid progress in the field of nonlinear optics. This article traces the history of materials development that has taken place over the past forty odd years and dwells on the current status in this important area. The materials aspect is discussed under three classes viz. inorganic, organic and semiorganic crystals. In the end, some of the crystal growth work that has been carried out in author's laboratory is presented.