Visible-light-activated photocatalysts based on samarium-doped, europium-doped, and gadolinium-doped nickel aluminates (SmNA, EuNA, GdNA) were synthesized. The spinel crystalline structures of the doped mixed metal oxides were demonstrated by X-ray diffraction (XRD) and transmission electron microscopy (TEM) analysis. The presence of the rare-earth metals (REMs) was confirmed by the energy-dispersive X-ray (EDX) studies. Ultraviolet-visible-near-infrared (UV-Vis-NIR) spectra revealed that the REMs-doped catalysts absorb in the full solar spectrum range covering both visible and near infrared wavelengths. Scanning electron microscopy (SEM) visualized the profound morphological alterations of the doped nickel aluminate samples. Consequently, the pore volume and the Brunauer-Emmett-Teller (BET) surface area decreased, while nanoparticles sizes increased. Fourier-transform infrared spectroscopy (FTIR) exposed that surfaces of REMs-doped nickel aluminates are rich in hydroxyl groups. Finally, the photocatalytic performance was notably increased through doping nickel aluminate (NA) with REMs; the highest activity was observed for EuNA.