[reaction: see text] Benzopyranoimidazolones could virtually exist in four tautomeric forms, namely N3-H, N1-H, coumarin O-H, and C2-H. Experimental evidence reported thus far has been unable to lead to a unique statement about the preferred tautomeric forms in solution. In this work, tautomeric equilibria for a series of 2-substituted [1]benzopyrano[3,4-d]imidazol-4(3H)-ones were investigated by DFT calculations, in both gas phase and solution. The influence of the solvent was included in the calculations by the CPCM solvent model. 13C chemical shifts of all tautomers were computed at different levels of theory and then compared with experiments to assign the preferred tautomers. Theoretical findings were then compared to dynamic 1H NMR experiments results.