New organic nonlinear optical crystal : dicyanovinyl anisole (DIVA) has been grown from vapor by low pressure sublimation and from saturated solution by solvent evaporation. Crystallographic structure and quadratic nonlinear optical properties were investigated. Molecular orientation in DIVA crystal with space group P21, is favorable for the highest possible value of bulk phase-matchable coefficient. Both type I and type II phase matched second harmonic generation (PMSHG) were observed from naturally grown faces of single crystals. Efficient PMSHG was achieved at a fundamental wavelength of 812 and 1064 nm. The efficient type I PMSHG coefficient was determined as deff = 4.9 × 10−8 esu = 40 × (d11 of α-quartz) at a wave.LH length of 1064 nm. Blue light generation was demonstrated by both PMSHG and sum-frequency mixing of the 812 nm laser with 1064 nm.