In this study, we systematically investigated the flux performance of ultrafiltration (UF) membranes functionalized with randomly-accumulated nanofibers. By electrospinning nanofibers from hydrophobic polysulfone (PSf) and hydrophilic cellulose (CL), we were able to explore the role that bulk nanofiber (NF) layer thickness, individual NF diameter, and intrinsic chemistry have on composite membrane flux. Additional parameters that we systematically tested include the molecular weight cut-off (MWCO) of the base membrane (10, 100, and 200 kDa), flow orientation (cross-flow versus dead-end), and the feed solution (hydrophilic water versus hydrophobic oil). Structurally, the crosslinked PSf nanofibers were more robust than the CL nanofibers, which lead to the PSfNF-UF membranes having a greater flux performance. To decouple the structural robustness from the water affinity of the fibers, we chemically modified the PSf fibers to be hydrophilic and indeed, the flux of these new composite membranes featuring hydrophilic crosslinked nanofibers were superior. In summary, the greatest increase in flux performance arises from the smallest diameter, hydrophilic nanofibers that are mechanically robust (crosslinked). We have demonstrated that electrospun nanofiber layers improve the flux performance of ultrafiltration membranes.