Electrospinning is a process by which polymer fibers can be produced using an electrostatically driven fluid jet. Electrospun fibers can be produced at the micro- or nano-scale and are, therefore, very promising for air filtration applications. However, because electrospun fibers are electrically charged, it is difficult to control the morphology of filtration media. Fiber size, alignment and uniformity are very important factors that affect filter performance. The focus of this project is to understand the relationship between filter morphology and performance and to develop new methods to create filtration media with optimum morphology. This study is divided into three focus areas: unimodal and bimodal microscale fibrous media with aligned, orthogonal and random fiber orientations; unimodal and bimodal nanoscale fibers in random orientations; bimodal micrometer and nanometer fiber media with orthogonally aligned orientations. The results indicate that the most efficient filters, which are those with the highest ratio of particle collection efficiency divided by pressure drop, can be obtained through fabricating filters in orthogonal layers of aligned fibers with two different fiber diameters. Moreover, our results show that increasing the number of layers increases the performance of orthogonally layered fibers. Also, controlling fiber spacing in orthogonally layered micrometer fiber media can be an alternative way to study the filtration performance. Finally, such coatings presented throughout this research study can be designed and placed up-stream, down-stream, and/or in between conventional filters.