Semi-interpenetrated polyvinyl alcohol polymer networks (SIPNs) were prepared by integrating various charged components into polyvinyl alcohol polymer. Contact angle measurement, attenuated total reflection Fourier transform infrared spectroscopy, field emission scanning electron microscopy, and tensile tests were used to characterize the physicochemical properties of the prepared SIPNs. To investigate the contribution of charges to marine antifouling, the adhesion behaviors of green algae Dunaliella tertiolecta and diatoms Navicula sp. in the laboratory and of the actual marine animals in field test were studied for biofouling assays. The results suggest that less algae accumulation densities are observed for neutral-, anionic-, and zwitterionic-component-integrated SIPNs. However, for the cationic SIPNs, despite the hydration shell induced by the ion–dipole interaction, the resistance to biofouling largely depends on the amount of cationic component because of the possible favorable electrostatic attraction between the cationic groups in SIPNs and the negatively charged algae. Considering that the preparation of novel nontoxic antifouling coating is a long-standing and cosmopolitan industrial challenge, the SIPNs may provide a useful reference for marine antifouling and some other relevant fields.