The invention relates to the field of utilization of coal ash acid-method extracted aluminum residues and coal ash, and discloses a method for preparing a 4A-type molecular sieve and a ZSM-5 (Zeolite Socony Mobil-5) molecular sieve from coal ash acid-method extracted aluminum residues and a use method of coal ash. The method comprises the following steps: (1) performing alkali roasting on the coal ash acid-method extracted aluminum residues so as to obtain a roasted residue material, performing high-temperature water leaching and heat-preservation filtration on the roasted residue material in sequence so as to obtain first filtrate; (2) performing 4A-type molecular sieve hydrothermal crystallization on the first filtrate so as to obtain a 4A-type molecular sieve and molecular sieve filtrate; and (3) performing ZSM-5 type molecular sieve hydrothermal crystallization on the molecular sieve filtrate, thereby obtaining the ZSM-5 molecular sieve and second filtrate. By adopting the method, elimination of the coal ash acid-method extracted aluminum residues can be achieved, the utilization rate of the coal ash acid-method extracted aluminum residues can be increased, and the utilization of the coal ash can be improved.