In this work, different methods for fly ash modification were applied to obtain an adsorbent for the efficient removal of selected pharmaceuticals from a multiclass aqueous solution. Morphological and surface properties of the modified fly ash samples were analyzed by scanning electron microscopy, X-ray fluorescence, X-ray diffraction, Fourier transform infrared spectroscopy, and point of zero charge, and the influence of the applied modifications was determined by comparison with the results obtained for unmodified fly ash. Experimental parameters of the adsorption of the pharmaceutical onto the modified fly ash were optimized, and special attention was paid to the influence of different parameters on the adsorption capacities. Multivariate methods of analysis, such as artificial neural networks, applied to the obtained results showed that the contact time, the initial concentration of the pharmaceutical solution, and the pH value had the strongest influence on the adsorption process. Fly ash modified with chitosan and magnetic iron oxide showed the best adsorption properties (removal efficiency above 80% for the majority of the selected pharmaceuticals), and artificial neural networks confirmed its susceptibility to the modeling process.