The present invention relates to the selective separation of hydrogen (“H2”) hydrocarbons in streams containing both hydrogen and hydrocarbons (e.g. methane, ethylene, ethane, propylene, propane, etc.) utilizing a zeolitic imidazolate framework (“ZIF”) material. Preferably, the stream to be separated is fed to the present process in a substantially gaseous phase. In preferred embodiments, the current invention is utilized in either a pressure swing adsorption process, a temperature swing adsorption process, or a membrane separations process to separate hydrogen from hydrocarbons present in hydrogen production streams or petrochemical/petroleum refining product streams and intermediate streams.