The recently popularized method of rotary jet spinning (RJS) or centrifugal spinning is investigated to evaluate the rheological limitations of polymer solutions and melts to optimal spinnability. The influence of Newtonian or non-Newtonian behavior of the polymer on spinnability is discussed. We observe that highly viscous polymers tend to block the die channels within a rotary jet spinneret and therefore suggest the use of relatively low Newtonian viscosities of between 1 and 10 Pa s for optimal fiber production. Computational fluid dynamics simulations are used in conjunction with experimental data to establish important processing parameters, such as typical shear rates in the device and optimal polymer melt or solution viscosities. A theoretical model for RJS is compared to measured fiber diameters. The comparison shows that although fiber diameters can be estimated very roughly in the case of polymer solutions, the prediction of fiber diameter in the case of polymer melts require further modeling work.