Li7La3Zr2O12 (LLZO) is a promising ceramic Li-ion conductor that has been successfully prepared in nanowire morphology using electrospinning from polymer/sol-gel solutions followed by calcination. However, conventional single-needle electrospinning has low production rates <0.1 g/h, making scale-up of the materials for applications in solid-state electrolytes challenging. Herein, needleless electrospinning using a twisted wire spinneret is employed to prepare Al-doped LLZO (ALLZO). We find that the appropriate precursor solutions for needleless electrospinning require much lower viscosity and are more sensitive to environmental conditions than those used in single-needle electrospinning. The as-formed nanofibers display a nanoribbon morphology, and calcination at 700 degrees C for 2 h in air results in phase pure ALLZO interconnected nanostructures with a cubic crystal structure. The results show that needleless electrospinning is an effective approach for preparing as-spun nanofibers with yields of similar to 1 g/h possible, providing a higher throughput route toward Li+ conducting nanostructures for solid-state battery applications.