Infrared spectroscopy and photometry with ISO covering most of the emission range of the interstellar medium has led to important progress in the understanding of the physics and chemistry of the gas, the nature and evolution of the dust grains and also the coupling between the gas and the grains. We review here the ISO results on the cool and low-excitation regions of the interstellar medium, where T gas≲ 500 K, nH ∼ 100–105 cm−3 and the electron density is a few 10−4.