Given the ever-increasing demand for gallium(III) as a crucial precursor in the fabrication of advanced materials, there arises an imperative to devise efficient recovery processes from primary and secondary sources. In the present investigation, the retrieval of gallium(III) from aqueous solutions through the mechanism of adsorption was investigated. Materials with superior adsorbent properties play an important role in the dynamics of the adsorption process. To enhance these properties, select materials, such as Amberlite-type polymeric resins, are amenable to functionalization through impregnation with extractants featuring specialized active groups, designed for the selective recovery of metal ions—specifically, Ga(III). The impregnation method employed in this study is the Solvent-Impregnated Resin (SIR) method, utilizing the amino acid DL-valine as the extractant. The new material was characterized through Scanning Electron Microscopy (SEM), Elemental Analysis via X-ray energy-dispersive spectroscopy (EDX), and Fourier transform infrared spectroscopy (FTIR) to elucidate the presence of the extractant on the resin’s surface. Concurrently, the material’s pHPZC was determined. The adsorptive prowess of the synthesized material was investigated through kinetic, thermodynamic, and equilibrium studies. The influence of specific parameters in the adsorption process—namely, pH, contact time, temperature, and Ga(III) initial concentration—on the maximal adsorption capacity was determined. The optimal adsorption conditions were established using the Taguchi method.