An object is to provide a method for producing a high theobromine-containing composition effectively in a simple way. The method for producing a theobromine-containing composition comprises: (a)performing an extraction of a theobromine-containing plant or a processed product thereof with a solvent, to obtain a crude theobromine extract (b) applying the crude theobromine extract to a cation exchange resin subjected in advance to hydrogen ion substitution, to allow an adsorption of theobromine onto the cation exchange resin and (c) passing a solvent containing no ionic substance through the cation exchange resin subsequently to the step (b), to obtain a theobromine eluate.