The determination of optical constants (i.e., real and imaginary parts of the complex refractive index (nc) and thickness (d)) of ultrathin films is often required in photonics. It may be done by using, for example, surface plasmon resonance (SPR) spectroscopy combined with either profilometry or atomic force microscopy (AFM). SPR yields the optical thickness (i.e., the product of nc and d) of the film, while profilometry and AFM yield its thickness, thereby allowing for the separate determination of nc and d. In this paper, we use SPR and profilometry to determine the complex refractive index of very thin (i.e., 58 nm) films of dye-doped polymers at different dye/polymer concentrations (a feature which constitutes the originality of this work), and we compare the SPR results with those obtained by using spectroscopic ellipsometry measurements performed on the same samples. To determine the optical properties of our film samples by ellipsometry, we used, for the theoretical fits to experimental data, Bruggeman’s effective medium model for the dye/polymer, assumed as a composite material, and the Lorentz model for dye absorption. We found an excellent agreement between the results obtained by SPR and ellipsometry, confirming that SPR is appropriate for measuring the optical properties of very thin coatings at a single light frequency, given that it is simpler in operation and data analysis than spectroscopic ellipsometry.