We characterized the thickness and surface damage layer of poly(methyl metacrylate) (PMMA) organic films irradiated with Ar cluster or monomer ion beam using ellipsometry. A heavily damaged layer was detected on the surface of the PMMA film irradiated with Ar monomer ion beam; more than 2–3 nm of the surface were completely metamorphosed into a carbon-like layer and damage had accumulated with irradiation. On the other hand, no significant damage was detected on PMMA films irradiated with Ar cluster ion beams. These results corresponded with measurements of the irradiated surface by X-ray photoelectron spectroscopy (XPS). The sputtering depth from PMMA film irradiated with Ar cluster/monomer ion beams can also be measured using the ellipsometry method at nanometer-order resolution. The optical method of ellipsometry may be a desirable tool for sputtering yield measurement and surface damage layer estimation for organic films.