The use of organic molecular crystals with large second-order nonlinear optical susceptibilities for implementing compact waveguide second-harmonic generation devices is addressed. The growth of metanitroaniline film crystal in a planar capillary with a channel/taper structure for single seed formation by zone melting recrystallization using a ridge heater is presented. Single-crystal film (5*15 mm/sup 2/, approximately 2- mu m thickness) was obtained with reproducible crystallographic orientation control. Cerenkov-radiation-type waveguide second-harmonic generation is demonstrated. >