The liquid-phase dehydration of 1,4-butanediol to tetrahydrofuran was investigated over various materials including synthetic zeolites, namely, ZSM-5, Y, Mordenite, Ferrierite, and Beta as well as silica and alumina. The key characters investigated were the Si/Al ratio and cation exchange. The results showed that the ZSM-5 zeolite exchanged with NH4+ exhibited the highest activity in dehydration of 1,4-butanediol. In all tests, nearly 100% selectivity to tetrahydrofuran was observed. After finding the most active catalyst, the kinetics of dehydration of 1,4-butanediol to tetrahydrofuran was studied over this material. The influence of operating parameters such as temperature, pressure, and substrate concentration on reaction was investigated through the Taguchi analysis of experimental data. A strong dependence of reaction rate on temperature was observed. Pressure, however, was found to have a negligible effect on reaction rate. The contribution of external and intraparticle mass transfer limitations on the overall reaction rate was negligibly small. A mechanism was proposed to explain the reaction rate. The proposed model could reasonably well predict the observed behavior.