The development of both “soft” and “hard” fabrication techniques for the patterning of nonlinear photonic devices in ionically self-assembled monolayer (ISAM) films is reported. A combination of electron beam lithography and reactive ion etching was used to pattern two-dimensional holes with a lattice of and diameters ranging from . A soft alternative to this fabrication was also demonstrated. Nanoimprint lithography was successfully employed to pattern similar photonic structures with average hole diameters of and a lattice spacing of , as well as Bragg gratings with a period of . Potential impact of this fabrication process on the chemical composition and nonlinear properties of the ISAM films was assessed using Fourier transform infrared spectroscopy, x-ray photoelectron spectroscopy, and second harmonic generation. The spectroscopy techniques confirmed that the chemical composition and bonding of the ISAM films was not adversely affected by the thermal cycles required for nanoimprinting. Second harmonic generation analysis also confirmed that the nanoimprinting process did not affect the nonlinear properties of the material, PCBS/PAH ISAM films, further indicating the suitability of such materials for the nanoimprinting of nonlinear optical photonic structures.