The worsening of air quality is an urgent human health issue of modern society. The outbreak of COVID-19 has made the improvement of air quality even more imperative, both for the general achievement of major health gains and to reduce the critical factors in the transmission of airborne diseases. Thus, the development of solutions for the filtration of airborne pollutants is pivotal. Electrospinning has gained wide attention as an effective fabrication technique for preparing ultrafine fibers which are specifically tailored for air filtration. Nevertheless, the utilization of harmful organic solvents is the major barrier for the large-scale applicability of electrospinning. The use of water-soluble synthetic polymers has attracted increasing attention as a ‘green’ solution in electrospinning. We reported an overview of the last five years of the scientific literature on the use of water-soluble synthetic polymers for the fabrication of multifunctional air filters layers. Most of recent studies have focused on polyvinyl alcohol (PVA). Various modifications of electrospun polymers have been also described. The use of water-soluble synthetic polymers can contribute to the scalability of electrospinning and pave the way to innovative applications. Further studies will be required to fully harness the potentiality of these ‘greener’ electrospinning processes.