A new aqueous and scalable strategy to synthesize surfactant-free Cu2Te nanotubes and nanosheets at room temperature has been developed. In aqueous solution, Cu2E (E = O, S, Se) nanoparticles can be easily transformed into Cu2Te nanosheets and nanotubes via a simple anion exchange reaction under ambient conditions. The formation of Cu2Te nanosheets is ascribed to a novel exchange-peeling growth mechanism instead of simple Kirkendall effect; and the resultant nanosheets can be further rolled into nanotubes with assistance of stirring. The morphologies of Cu2Te nanosheets and nanotubes can be easily controlled by changing the synthesis parameters, such as the concentration of precursors, the size of nanoparticle precursor, and the amount of NaBH4, as well as the stirring speed. Thus-formed Cu2Te nanostructures exhibit excellent catalytic activity toward sulfide redox shuttles and are exploited as counter electrodes catalysts for quantum dot sensitized solar cells. The performance of Cu2Te nanostructures strongly depends on their morphology, and the solar cells made with counter electrodes from Cu2Te nanosheets show the maximum power conversion efficiency of 5.35%.