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Density functional theory (DFT) and ab initio calculations were performed to probe the origin of the magnetic relaxation barriers for two finite single-chain magnets (SCMs) featuring a one-dimension chain, Chfac)2(R-NapNIT) (R-NapNIT = 2-(2'-(R-)naphthyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide, R = MeO (1) or EtO (2)). Our calculations show that the strong intrachain CoII-CoII exchange coupling interactions transmitted by radicals can contribute much more than ionic anisotropy to the height of the reversal barrier of magnetiza
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