Anthracene and polyethylene thin films were deposited by ionized cluster beam (ICB). Films deposited at optimum ion acceleration voltage showed strong preferential crystal orientation. The dependencies of crystal orientation and film grain size on deposition conditions were investigated. The photoluminescent and electroluminescent properties of anthracene films deposited by ICB were superior to those properties of similar films produced by vacuum deposition. In the case of polyethylene, it was found that in films produced by ICB, the molecules contain fewer side chains than in the source material. The lattice parameter in ICB polyethylene films was close to that of the single crystal polyethylene material. Strength of film–substrate adhesion was improved by increasing ion acceleration voltage.