In the past few decades, the role of nanotechnology has expanded into environmental remediation applications. In this regard, nanofibers have been reported for various applications in water treatment and air filtration. Nanofibers are fibers of polymeric origin with diameters in the nanometer to submicron range. Electrospinning has been the most widely used method to synthesize nanofibers with tunable properties such as high specific surface area, uniform pore size, and controlled hydrophobicity. These properties of nanofibers make them highly sought after as adsorbents, photocatalysts, electrode materials, and membranes. In this review article, a basic description of the electrospinning process is presented. Subsequently, the role of different operating parameters in the electrospinning process and precursor polymeric solution is reviewed with respect to their influence on nanofiber properties. Three key areas of nanofiber application for water treatment (desalination, heavy-metal removal, and contaminant of emerging concern (CEC) remediation) are explored. The latest research in these areas is critically reviewed. Nanofibers have shown promising results in the case of membrane distillation, reverse osmosis, and forward osmosis applications. For heavy-metal removal, nanofibers have been able to remove trace heavy metals due to the convenient incorporation of specific functional groups that show a high affinity for the target heavy metals. In the case of CECs, nanofibers have been utilized not only as adsorbents but also as materials to localize and immobilize the trace contaminants, making further degradation by photocatalytic and electrochemical processes more efficient. The key issues with nanofiber application in water treatment include the lack of studies that explore the role of the background water matrix in impacting the contaminant removal performance, regeneration, and recyclability of nanofibers. Furthermore, the end-of-life disposal of nanofibers needs to be explored. The availability of more such studies will facilitate the adoption of nanofibers for water treatment applications.