The optical and photocatalytic properties of yttrium and lanthanum aluminates obtained by Pechini sol-gel process were studied by comparison. The aluminates were characterized by XRD, TEM, SEM, DRS, FTIR and PL spectroscopy. The photocatalytic properties were investigated in the removing of both cationic and anionic dyes from aqueous solutions. A higher photocatalytic activity was identified for yttrium aluminate (90% - 97% after 90 min), with the maximum value for methylene blue solution (97.15%), and a photocatalytic activity of 46.88% was determined for lanthanum aluminate in the degradation of methylene blue. The photocatalytic activity was in a good correlation with the aluminates optical behavior.