2-Acylamino-6-[1H]-pyridones [acyl= RCO, where R= methyl (1), ethyl (2), iso-propyl (3), tert- butyl (4), and 1-adamantyl (5)] have been synthesized and characterized by NMR spectroscopy. From three congeners, 2, 3 and 5, also single crystal X-ray structures have been solved. For these derivatives GIPAW calculations acts as a “bridge” between solid- state NMR data and calculated chemical shifts based on X-ray determined geometry. In ...