The interaction of pyrrole with alkali metal ion exchanged ZSM-5 (Li+, Na+, K+, Rb+, and Cs+) was studied by the combination of FTIR spectroscopy and the computational hybrid quantum mechanics/interatomic potential function method describing the role of the aluminum framework content and aluminum distribution, pyrrole coverage, cation size, and cation coordination type. The experimental spectral characteristics were explained using the comparison with the results of computational study. The pyrrole interaction with the metal cation (Lewis acid site) is driven by the pyrrole ring interaction with the metal cation, and it is further stabilized by the formation of a hydrogen bond of the pyrrole NH group with the framework oxygen atom. A large shift of NH vibrations to lower frequencies upon the pyrrole adsorption in M+/ZSM-5 observed experimentally is almost entirely due to the formation of a hydrogen bond. Two types of the pyrrole NH hydrogen bond were identified: the hydrogen bond to the oxygen atom of the Al-O-Si framework sequence and the hydrogen bond to the oxygen of the Si-O-Si framework sequence. The former type of hydrogen bond shows a larger red shift (\Deltav\ > 150 cm(-1)) and corresponds to a broad shoulder in the IR spectra whereas the latter type of hydrogen bond shows a moderate red shift (80 < \Deltav\ < 150 cm(-1)) and it corresponds to the band maximum. The shape of the IR spectra depends on the Si/Al ratio, alkali metal ion size, and pyrrole coverage. The combination of experimental and computation approaches brings a new insight into the interaction of pyrrole with alkali metal exchanged ZSM-5 and it provides interpretation of IR spectra at the atomic scale level.