Transparent and high moisture barrier acrylic coatings were obtained by deposition of acrylic resin containing crosslinking agents onto cellulose ester films, followed by exposure to atmospheric plasma. The effects of monomers, crosslinking agents, and polymerization methods were studied. The surface chemical composition, morphology, water vapor transmission rate (WVTR), light transmittance, and adhesion performance of the coated cellulose triacetate (CTA) films were characterized for the acrylic coated films and for different plasma treatments. Coated films showed a significant reduction in water vapor permeability while maintaining excellent transparency when compared with uncoated films. Furthermore, adhesion of the coating to the CTA film was also improved due to plasma treatment. It was also found that plasma curing on the coated oligomers can induce morphological changes and significantly increase surface roughness and hydrophilicity. The roughness texture observed via SEM analysis indicated that the types of plasma polymerization and the amount of crosslinking agents control the texture types for acrylic coating. Plasma-assisted acrylic coated CTA films can be used in electronic displays, medical, and packaging applications.