Recently,v arious titanium dioxide (TiO 2)n anostructures have received increasing attention in the fields of energy conversion and storage owingt ot heir electrochemical properties.H owever,t hese particulate nanomaterials exclusively exist in the powder form, which may cause health risks and environmental hazards.H erein we report an ovel, highly elastic bulk form of TiO 2 for safe use and easy recycling. Specifically,T iO 2 nanofibrous aerogels (NAs) consisting of resiliently bonded, flexible TiO 2 nanofibers are constructed, which have an ultralowb ulk density,u ltrahigh porosity,a nd excellent elasticity.T op romote charge transfer,t hey are subjected to lithium reduction to generate abundant oxygen vacancies,whichcan modulate the electronic structure of TiO 2 , resulting in ac onductivity up to 38.2 mS cm À1 .A saproof-ofconcept demonstration, the conductive and elastic TiO 2 NAs serve as an ew type of self-supported electrocatalyst for ambient nitrogen fixation, achieving an ammonia yield of 4.19 10 À10 mol s À1 cm À2 and aF aradaic efficiency of 20.3 %. The origin of the electrocatalytic activity is revealed by DFT calculations.