Adsorptive filtration is a technique based on the coating of a filter medium with adsorbents, resulting in modified media that can act simultaneously as a filter and as an adsorbent. Numerous studies have demonstrated that adsorptive filtration is a promising technology for removal of inorganic and microbiological contaminants. While previous studies have demonstrated the ability to coat granular media by precipitation of metallic salts, this study applied nanoscale materials as coatings. This study involved the development of an innovative physicochemical adsorptive filtration technology for removal of bacteriophage MS2 and arsenic in groundwater. The effects of pH and coating density on contaminant removal were evaluated through coated and uncoated anthracite and granular activated carbon. Lowering pH and increasing coating density resulted in higher arsenic and MS2 removal. This study not only demonstrated the benefits of nanoparticulate aluminum oxide coated filter media but also characterized the potential risks associated with their implementation.