We have devised an indirect laser-heated pedestal growth method to obtain organic nonlinear optical (NLO) devices with high wavelength conversion efficiency through the second-order NLO effect of materials. Using the method, the growth direction of organic NLO crystal can be controlled and a long interaction length in the phase-matched direction is attained. As an organic NLO crystal, 2-adamanthylamino-5-nitropyridine (AANP) has been grown and its optical properties are characterized. The results show that Type II angle-tuned phase-matched wavelength conversion is possible in the wavelength region from 1.2 to 1.7 μm. To reduce the absorption of the AANP crystal in the 1.55 μm wavelength region, we have fabricated deuterated derivartives of AANP and succeeded in increasing the wavelength conversion efficiency.