The aim of this study was the electrospinning of zirconia nanofibers without sol-gel precursors. Low-cost Zr-oxide and Zr-carbonate inorganic materials, with high molecular Zr-content compared to sol-gel methods, were used for precursor formulation. Using a polyvinylpyrrolidone (PVP) polymeric binder, zirconia nanofibers could successfully be synthesised with both Zr-sources. The effects of different electrospinning parameters were investigated to stabilize the processing and reduce the deviation of nanofiber diameters. Fibres calcined at 1000 °C produced from the two different precursors displayed differing crystal phases of zirconia. The one based on nanoparticles revealed a significantly higher amount of tetragonal phase. Zirconia nanofibers with poly-granular microstructure across the diameter were successfully produced.