In the present study, positively charged graphene oxide (GO) was prepared by a simple method under mild reaction conditions. The samples were characterized via Zeta potential, Fourier transform infrared spectroscopy, Raman spectroscopy, X-ray diffraction, and Scanning electron microscope. The results showed that GO was successfully modified by Poly (diallyldimethylammoniumchloride) (PDDA). The obtained sample (PDDA-GO) still had a lamellar structure; however, it clearly presented wavy wrinkles appearance in the surface microscopy morphology. When the ratio of GO to PDDA was 1:13, the fabricated PDDA-GO sheets possessed a high positive charge value and a good dispersion in water. Also, to study the interaction between PDDA and GO in PDDA-GO, GTA modified GO was selected as a comparative experiment. The Fourier transform infrared spectroscopy, UV/vis spectroscopy, and Fluorescence spectroscopy results indicate that the π-π interactions played a leading role in the process of PDDA modified GO sheets. While the electrostatic interactions played an inferior role in the same process.