Adding nanoparticles into polymer solutions before electrospinning creates unique hierarchical morphologies dispersed throughout small diameter nanoparticle-polymeric fibers. Effects of polymer composition, nanoparticle (NP) type, loading, and electrospinning voltage conditions were studied. As examples, indium, iron, and titanium oxide engineered nanoparticles (NPs) were dispersed into polyvinylpyrrolidone or polystyrene and electrospun. NP loadings below 5 wt % did not affect critical voltage required for Taylor cone formation, whereas higher NP loadings require higher critical voltages. Polymeric fiber thickness and macroscopic morphology is not impacted by up to 5 wt % NP loadings, and NP dispersion throughout the fibers were similar to their dispersion in initial polymer suspension. NP loadings above 5 wt % increased viscosity, which decrease subsequent fiber diameter. Experiments in water containing inorganic and organic pollutants in water demonstrate that the polymer is largely nonporous. This work enables design of multifunctional nanomaterial-polymer composite fibers for wide-ranging applications such as water and air treatment. (C) 2016 Wiley Periodicals, Inc.