Copolymer thin films of isoprene with acrylic acid were synthesized using PECVD. In that way, the stretchable functionality of polyisoprene (PI) was combined with the hydrophilic functionality of poly(acrylic acid) (PAA) to obtain stretchable thin films with adjustable wettabilities. Deposition rates were found to change between 9 and 5.5 nm/min depending on the monomer flowrates. The analysis of water contact angle (WCA) values indicated that films having more AA units in their structures were more wettable. The stretchability of the films was assessed on laboratory gloves through stretch-release test and on PET sheet through bend-release test. No significant changes in the WCA values with no observable cracks and failures after successive tests were indication of stretchability of the copolymer films.