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A highly efficient synthesis of carbamoylated benzimidazo[2,1-a]isoquinolin-6(5H)-ones using 2-arylbenzoimidazoles and oxamic acids was developed. This strategy tolerated various substrates as the starting materials to generate the corresponding products in good yields under metal-free conditions.Low-temperature heat capacity analyses for an NO-encapsulated fullerene derivative revealed (i) low-energy motion and (ii) strong magnetic anisotropy of the NO molecule due to its orbital angular momentum. The low-energy motion was attributed to