Mechanical alloying and annealing at 1023 K for 0.5 h under an argon atmosphere were used to prepare Ti2Ni-based nanocrystalline alloys and their nanocomposites. Ti2Ni alloy was chemically modified by Pd and multi-walled carbon nanotubes. An objective of the present study is to provide data on hydrogenation properties of Ti2Ni-based alloys and compounds containing Pd and/or multi-walled carbon nanotubes. Alloys and composites were characterized by X-ray diffraction, scanning electron microscopy equipped with an electron energy dispersive spectrometer, transmission electron microscopy, atomic force microscopy to evaluate phase composition, crystal structure, grain size, particle morphology and distribution of catalyst element. Hydrogenation/dehydrogenation properties and hydriding kinetics of materials were measured using a Sievert's apparatus. Hydrogenation properties of nanostructured Ti2Ni-based alloy and Ti2Ni-based nanocomposites were compared with those of the binary Ti2Ni compound. In present work we shown how mechanical alloying method and chemical modification by Pd and MWCNTs affected hydrogen storage properties of Ti2Ni alloy. The highest hydrogen capacity obtained for nanostructured Ti2Ni + Pd alloy equaled 2.1 wt.%. Up to our knowledge it is the highest hydrogen storage capacity obtained so far for Ti2Ni-based materials.