Sulfonatcd C-60, 5,10,15,20-tetra kis 4-[meso-tetra-methyl (4-pyridinyl)] porphyrin (C-60(SO3-)(n)-TMePyP4+) complex films have been prepared by electrostatic self-assembly of each chromophore from solution. When these complex films are formed on a thin film of chitosan polymer, the stacked bilayer films exhibit nearly twice the absorption as those prepared on conventional silanized substrates. X-ray photoelectron spectroscopy measurements disclose a strong interaction between the C-60(SO3-)(n) and TMePyP4+. Atomic force microscopy results of the surface morphology, hardness, and the chemical functionality are used to explain the differences between substrate treatments.