A stable monolayer assembly of octadecylcytosine, which can not be spread as a monolayer on pure water subphase, was formed when a small amount of guanosine was added to the water subphase. Spiral shaped two-dimensional crystal domains of the monolayer were observed by a fluorescence microscope. Fourier transform IR spectrum of the deposited monolayer prepared on the guanosine subphase strongly suggests complementary base pairing at the interface.