The application of (picosecond) nonlinear infrared spectroscopy to investigate zeolite catalysts and adsorbates is reviewed. In these time-resolved experiments, one specific vibration in the zeolite system (i.e., a zeolite or adsorbate vibration) is selectively excited with an ultrashort (tunable) mid-infrared pulse. The effect of this excitation and the subsequent energy relaxation can be monitored real time, providing information on the structure of the bare zeolite and adsorption complexes. More importantly, with this technique the picosecond energy flow at the catalytic site and thedynamicsof the catalyst-adsorbate interaction can be investigated: Short-lived transient species (e.g., reaction intermediates) are observed and the picosecond relaxation rates and pathways at the catalytic site render insights into the dynamics of the interaction between the zeolite catalyst and its adsorbates at a molecular level. This illustrates the potential of time-resolved infrared spectroscopy in the investigations of catalytic systems.