This study’s aim is a comparison of the plasma-induced effects on polymers exposed in helium and argon gaseous environments in a pulsed dielectric barrier discharge at atmospheric pressure. Cellulose-based and synthetic polymers are tested with regard to a range of parameters, such as wettability, adhesion, surface energy and polarity, the oxygen amount in their structure, and surface morphology. The surface properties are analyzed by contact angle measurements, X-ray photoelectron spectroscopy, and scanning electron microscopy images. The results point to the efficient and remarkably stable modifications of the plasma-exposed surfaces, such as their enhanced adhesion, surface energy, and oxygen incorporation. Additionally, plasma provides significant oxygen uptake in cellulose-based materials that bear already prior to treatment a high amount of oxygen in their structure. The comparison between the properties of the non-permeable, homogeneous, smooth-surface synthetic polymer and those of the loosely packed, porous, heterogeneous cellulose-based polymers points to the different rates of plasma-induced modification, whereby a progressive alteration of cellulosic surface properties over much larger ranges of exposure durations is noted. Present experimental conditions ensure mild treatments on such sensitive material, such as paper, and this is without alterations of the surface morphology and the physical degradation of the material over a large range of treatment duration.