In this study the wetting characteristics of untreated and plasma-treated polyurethane thin films were investigated. The degree of wettability was investigated by measuring the contact angle formed between a liquid drop and the solid surface. The work of adhesion, interfacial free energy, spreading coefficient, and Girifalco–Good's interaction parameter changed significantly for plasma-treated polyurethane films. Both complete and partial wetting were analyzed from the spreading coefficient of liquid drops on the solid substrate.