An attractive and challenging approach to the construction of robust, thin film materials with large second-order optical nonlinearities is the covalent self-assembly of aligned arrays of high-β molecular chromophores into multilayer superlattices. In this paper, we describe the dispersion of second harmonic generation (SHG) in a self-assembled (SA) monolayer containing a stilbazolium chromophore. The frequency-dependent measurements were performed on 25 Å thick monolayers on glass using a tunable (0.4–2 μm) light source based on optical parametric amplification (OPA). The SHG spectrum contains a clear two-photon resonance at hω = 1.3eV. The maximum in the second-order susceptibility coincides with a low energy chromophore-centered charge-transfer excitation at 480 nm. The experimental SHG dispersion values compare favorably with theoretical results computed using a sum-over-states (SOS) formalism. However, the measured values exhibit a somewhat broader band response than the theoretical curve, and the origin of this behavior is discussed.