Coal gangue is a kind of solid waste produced in the process of coal mining and washing. Its silicon aluminum silicon aluminum oxide content is high, respectively, which are suitable for resource utilization as raw materials for Si–Al molecular sieving. In this paper, a novel, simple, low-cost, and environmentally friendly process was carried out to prepare ZSM-5 zeolite by solvent free method after calcination, acid leaching, and alkali melting. The obtained samples were characterized by Energy Dispersive Spectrometer (EDS), Inductively Coupled Plasma (ICP), Thermo-gravimetry Analysis (TG), X-ray Photoelectron Spectroscopy (XPS), Fourier Transform Infrared Spectrometer (FTIR) X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM) and N2 adsorption isotherm. The characteristics of the raw materials and the adsorption mechanism of the prepared samples were characterized. Through a series of pretreatment such as calcined acid leaching and alkali melting of the raw materials, the silicon-aluminum ratio of the sample reaches 1.749, and the maximum specific surface area of the sample can reach 252.59 m2/g. The obtained samples were used to adsorb heavy metal ions and methylene blue solution, and the removal rate of lead ions and methylene blue solution was more than 95%. The theoretical maximum adsorption capacity of Pb ion, methylene blue solution and copper ion can reach 232.56 mg/g and 118.34 mg/g. The adsorption process is mainly chemical adsorption. The product could be suitable for removing both heavy metal ions and cationic dyes from the wastewater and had broad application prospects. Display omitted •The raw coal gangue was pretreated by calcination, acid leaching and alkali melting to concentrate silicon to improve the silicon-aluminum ratio.•ZSM-5 molecular sieve was prepared by solventless grinding method, which is an energy saving and environmental protection method.•The adsorption of heavy metal ions and methylene blue molecules in samples is mainly chemisorption, and the adsorption process is stable, and the cyclic adsorption effect is good.