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13C and 15N NMR Study of Electron Distribution in N‐Aryl‐N′‐cyanoguanidines

13C and 15N NMR spectroscopic assignments are given for a series of N‐aryl‐N′‐cyanoguanidines in DMSO‐d6 along with those for a few related cyanoguanidines. The NMR data are interpreted in terms of minimal overlap of the amino lone pair with the attached aryl ring, and a planar guanidine structure with the three nitrogen and one carbon pz orbitals forming a delocalized π‐orbital analogous to the guanidinium ion structure; the N‐aryl and the N′‐cyano groups act as π‐inductive substituents to the system.