This review considers the use of poly(alkylcyanoacrylates) (PACAs) as biomedical materials. We first present the different aspects of the polymerization of alkylcyanoacrylate monomers and briefly discuss their applications as skin adhesives, surgical glues and embolitic materials. An extensive review of the developments and applications of PACAs as nanoparticles for the delivery of drugs is then given. The methods of preparation of the nanoparticles are presented and considerations concerning the degradation, in vivo distribution, toxicity and cytotoxicity of the nanoparticles are discussed. The different therapeutic applications are presented according to the route of administration of the nanoparticles and include the most recent developments in the field.