We have investigated olefins adsorbed on Bronsted acidic hydroxyl groups (OD) of DM20 zeolite by transient infrared absorption spectra after excitation of the OD stretching mode using picosecond infrared lasers. The olefins studied were ethylene, deuterated ethylene, propylene, and isobutene, and only isobutene was adsorbed on OD at its methyl group while the other olefins were adsorbed at their double bonds. For all the olefins except isobutene, simple vibrational relaxation of the v = 1 state was observed and the lifetimes were 2-4 ps. These lifetimes are an order faster than that of isolated OD. For isobutene, a long lifetime component lasting more than 500 ps was observed in addition to vibrational relaxation of 2 ps. The transient absorption spectra for isobutene-adsorbed zeolite at various time delays and frequencies indicated the existence of a short-lived species and a slow desorption process compared with vibrational relaxation.