The solvent-free, microwave-assisted 1,3-dipolar cycloaddition of carbonyl ylides, generated from a series of oxiranes, to SWCNTs (single-walled carbon nanotubes) is described. The procedure is extremely fast and repeatable. The reaction of SWCNTs with benzylidenmalononitrile epoxide afforded a gem-dicyano derivative that is well-suited to further transformation into esters or amides through the Pinner reaction.