3-Acetylpyridine (AcP), as an organic hydrogen carrier, and Pd nanoparticles, as a catalyst, were incorporated into MIL-101(Cr) for chemical hydrogen storage. AcP was first grafted into MIL-101(Cr), and then Pd (0.5-4.0 wt %) was encapsulated by a double-solvent adsorption process. Thermogravimetric analysis, inductively coupled plasma-optical emission spectrometry, X-ray photoelectron spectroscopy, transmission electron microscopy, in situ X-ray adsorption near-edge structure analysis, H-1 nuclear magnetic resonance (NMR), and elemental analysis suggested the existence of AcP and Pd nanoparticles (NPs) inside the MIL-101(Cr) cages. The chemical hydrogen storage of samples was evaluated by H-2 temperature-programmed reaction. In situ Fourier transform infrared and H-1 NMR techniques verified the hydrogenated and dehydrogenated forms of AcP upon hydrogen uptake. Reversible hydrogenation/dehydrogenation can be readily regulated by H-2 partial pressure and temperature. The chemical hydrogen storage could be accomplished only when AcP and Pd NPs were adjacently present. The chemical hydrogen storage was enhanced with an increased Pd loading up to 0.33 mmol H-2.g(-1) per cycle. With the manipulation of hydrogenation and dehydrogenation temperatures at 150 degrees C, the chemical hydrogen storage can be maintained for up to 10 cycles. The material reported herein is one of the noncryogenic chemical hydrogen storages that can be operated at constant temperature and atmospheric pressure.