This paper investigated the influence of various processing parameters of atmospheric pressure plasma jet (APPJ) on the etching behavior of PVA films. The etching rate increased as output power, and moisture regain increased. As the treatment time increased, the etching rate increased initially and then decreased. Atomic force microscopy (AFM) results showed that the surface roughness varied as the moisture regain (MR) (2.45%, 9.32%, and 78.31%, respectively) of PVA films changed during APPJ treatment. It was found that higher moisture regain and lower thermal conduction of underlayer had negative effect on the solubility of plasma treated PVA films.