In this paper, atmospheric pressure plasma of ambient air was generated by a surface dielectric barrier discharge (SDBD) device for the purpose of modifying the surface of isotactic-polypropylene (iPP). The effect of SDBD treatment time on the chemical and physical properties of iPP was studied using various analytical techniques including, water contact angle (WCA), attenuated total reflection (ATR), Raman spectroscopy, x-ray diffraction (XRD), and atomic force microscopy (AFM). The results indicate that the hydrophilicity and the C=O bonds of the treated iPP were improved as observed, respectively, through WCA and ATR analysis. The crystal structure was evaluated by Raman spectroscopy and XRD. It was found that the iPP chain was under microscopic stress, which affected its crystallinity degree depending on the duration of the treatment. Furthermore, the AFM analysis revealed that the surface roughness was substantially modified.