The invention provides a comprehensive utilization method of hydrargillite-produced 4A zeolite waste residue. The method comprises the steps of: separating the ferrosilicoaluminum component in the hydrargillite-produced 4A zeolite waste residue by means of acid leaching and filtering, wherein the obtained mixed liquor of filter liquor and filter residue washing liquor is used for preparing a polymeric aluminum ferric chloride water purifying agent; and removing iron from the wet slag obtained by washing the filter residue by means of alkali fusing, roasting and activating, and synthesizing the 4A zeolite by a hydrothermal method by means of adjusting and assembling. Triethanolamine is taken as a complexing agent of the microelement iron in the liquor during synthesizing the 4A zeolite, sothat the produce of an iron precipitate is overcome, and the whiteness of a 4A zeolite product is guaranteed; sodium sulfide is reacted with a triethanolamine iron complex in the zeolite-synthesized mother liquor to reduce the triethanolamine and obtain an iron sulfide precipitate; and removing the mother liquor of the iron sulfide precipitate to realize the cycle utilization. The synthesis method of the 4A zeolite adopts a sealed cycle technology, thereby being stable in operation, and free of the generation of new waste liquor and new waste slag.