Alkyl 2-cyanoacrylates (CAs) are primarily used as instant adhesives, including those sold under the Loctite brand. The adhesive action can be inhibited with acid stabilizers allowing radical polymerization to be employed. The following article details the first attempted controlled/living radical polymerization of alkyl CAs: Reversible addition fragmentation chain transfer (RAFT) polymerization mediated by a poly (methyl methacrylate) dithiobenzoate macroRAFT agent for three different CA monomers (ethyl 2-cyanoacrylate, n-butyl 2cyanoacrylate, and 2-phenylethyl cyanoacrylate) allowed the preparation of the first block copolymers of this challenging but commercially important monomer class. Nevertheless, GPC with UV detection indicated significant loss of the RAFT end-group for all three CAs limiting control/living character. VC (C) 2017 Wiley Periodicals, Inc.