A range of chemical pollutants is present in drinking water sources, including organic compounds, (e.g., pharmaceuticals and pesticides) and heavy metals (e.g., arsenic and lead). To protect the health of consumers, particularly those with private drinking water wells and in urban areas with aging water distribution systems, drinking water treatment at the point of use (POU) is essential. Next-generation POU technologies must require minimal energy, efficiently remove a range of pollutants, and be simple enough to permit broad application across users. Nanomaterials are ideal candidates for such technologies, as they exhibit high reactivity within small physical footprints. However, concerns regarding pressure requirements and material release challenge their application in traditional reactor designs. To bridge the gap between potential and practical application of nanomaterials, this study utilizes electrospinning to fabricate composite nanofiber filters. In electrospinning, a high voltage draws a polymer precursor solution (which can contain nanomaterial additives) from a needle, depositing a non-woven nanofiber filter on a collector. Using electrospinning, we develop an optimized carbon nanotube-carbon nanofiber composite that achieves a key balance between material strength and reactivity towards organic pollutants. Additionally, we develop two optimized polymer nanocomposites with embedded iron oxide nanoparticles and/or ion exchange groups, and demonstrate their application for removal of a range of metal contaminants (e.g., arsenic, chromium, lead, copper, and cadmium). Outcomes of this work establish novel methods for nanocomposite fabrication, contributing to the responsible and effective deployment of nanomaterials in POU drinking water treatment.