To examine the feasibility of developing multifunctional textiles, layered fabric systems with electrospun polyurethane/zinc oxide nanocomposite fiber webs layered on cotton substrates were developed to impart UV‐protection and antibacterial functions. The morphology of polyurethane/zinc oxide nanocomposite fibers was examined using a field‐emission scanning electron microscope and a transmission electron microscope. UV transmission properties were assessed for layered fabric systems with various levels of electrospun web area density. Antimicrobial properties of zinc oxide nanocomposite fibers and layered fabric systems were evaluated qualitatively using the Parallel Streak method, and quantitatively by measuring the bacterial reductions of a Gram‐positive bacterium (Staphylococcus aureus) and a Gram‐negative bacterium (Klebsiella pneumoniae). A thin layer of electrospun zinc oxide nanocomposite fiber web significantly reduced the transmission of UV radiation and exhibited an ultraviolet protection factor of greater than 50, indicating excellent UV protection. Layered fabric systems with zinc oxide nanocomposite fiber webs containing 5 wt % zinc oxide exhibited over 98% reduction in both Staphylococcus aureus and Klebsiella pneumoniae. The results show that the successful imparting of multifunctionalities such as UV‐protection and antibacterial functions to cotton fabrics is achievable through simultaneous electrospinning of the polymer material with zinc oxide nanoparticles. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009