A comprehensive theoretical study of the hydrogen bonding interactions and microscopic solvation structures of a pyridyl-urea-based hydrogelator in aqueous solution

► DFT calculations and MD simulations were performed. ► N,N′-bis(4-pyridyl) urea is significantly polarized in aqueous solution. ► Specific O⋯HO, N⋯HO, and NH⋯O hydrogen bonding interactions coexist in aqueous solution. ► DFT and MD simulation have their own advantages and limitations. ► The theoretical results explain why N,N′-bis(4-pyridyl) urea can act as a hydrogelator.