We report grating-coupled surface plasmon resonance measurements involving the use of dispersion images to interpret the optical response of a metal-coated grating. Optical transmission through a grating coated with a thin, gold film exhibits features characteristic of the excitation of surface plasmon resonance due to coupling with the nanostructured grating surface. Evidence of numerous surface plasmon modes associated with coupling at both front (gold/air) and back (gold/substrate) grating interfaces is observed. The influence of wavelength and angle of incidence on plasmon coupling can be readily characterized via dispersion images, and the associated image features can be indexed to matching conditions associated with several diffracted orders at both the front and back of the grating. These features collapse onto a set of global dispersion curves when plotted as peak energy versus the grating wavevector, with feature locations clustered according to the refractive index values of the neighboring dielectric material, either air or polycarbonate. Coating of the grating with multilayer arachidic acid films via Langmuir–Blodgett deposition results in red-shifting of some, but not all, of the plasmon features. The magnitude of the shift is a function of the film thickness, wavelength, and angle of incidence. Dispersion images clearly depict the red-shifting and also broadening of the front side features with increasing film thickness. In contrast, little change is observed in features associated with the back-side of the grating. The nature and magnitude of the interaction between the plasmon modes appearing at the front and back sides of the grating are discussed and analyzed in terms of the predicted interactions determined via optical modeling calculations.