Polymers are versatile compounds which physical and chemical properties can be taken advantage of in wide applications. Particularly, in the biomedical field, polydimethylsiloxane (PDMS) is one of the most used for its high biocompatibility, easy manipulation, thermal, and chemical stability. Nonetheless, its hydrophobic nature makes it susceptible to bacterial pollution, which represents a disadvantage in this field. A potential solution to this is through the graft of stimuli-sensitive polymers that, besides providing hydrophilicity, allow the creation of a drug delivery system. In this research, PDMS was grafted with acrylic acid (AAc) and vinyl pyrrolidone (VP) in two steps using gamma radiation. The resulting material was analyzed by several characterization techniques such as infrared spectroscopy (FTIR), swelling, contact angle, critical pH, and thermogravimetric analysis (TGA), demonstrating the presence of both polymers onto PDMS films and showing hydrophilic and pH-response properties. Among the performed methods to graft, the loading and release of ciprofloxacin were successful in those samples obtained by direct irradiation method. Furthermore, the antimicrobial assays showed zones of inhibition for microorganisms such as Staphylococcus aureus and Escherichia coli.