A facile sol-gel method was used to synthesize an innovative nanocomposite containing Terbium orthoferrite (TbFeO3) and Terbium orthocobaltite (TbFeO3) with olive and Vitex agnus-castus leaves as natural reduction agents. The desired product comprised of two perovskites, TbFeO3 and TbCoO3, was utilized to degrade two anionic and cationic dyes after optimizing the synthesis conditions. A better photocatalytic efficiency in acidic media may be achieved as a result of the better performance of this nanocomposite for degradation of anionic dye. Also, the two other reactions were performed separately in order to synthesize each of the components of the as-synthesized nanocomposites. A couple of three-component nanocomposites with fascinating properties were produced as a result of this experiment. As a result of optical studies, different patterns of charge carrier transfer were assumed for them, which contributed to the theoretical creation of heterojunction photocatalysts with a variety of configurations. A summary of the results shows that the maximum degradation percentage of Eriochrom Black T during 90 min under visible light in pH = 5 in the presence of as-prepared was 91.7. This two-component nanocomposite demonstrated a type I configuration for charge carrier transfer.