A Cu(OTf)(2)-catalyzed and TsNCO-mediated three-step tandem synthesis of 9-arylfluorenes were developed from biphenyls and aryl aldehydes, by which the electron-poor 9-aryl substituted fluorenes were synthesized smoothly. Its success is mainly attributed to use an anhydrous synthesis of N-tosyl arylaldimines as a key step, which was achieved in situ from the reaction of TsNCO and aryl aldehydes. (C) 2016 Elsevier B.V. All rights reserved.