Herein, a novel and stable Tb-Co-O nanocomposite photocatalyst is fabricated through a one-pot microwave route for 2 min (600 W, 20 s On, 60 s Off), which is introduced as UV/Visible light active catalysts in wastewater treatment. Employing various combined parameters of Tb:Co ratio, pH adjustment agents, chemical and natural templates, the resulting nanostructures displayed the intrinsic structure nature, narrow size distribution, good optical properties, and excellent photocatalytic efficiency. The formation of Tb-Co-O nanostructures and their features were verified via X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), and ultraviolet–visible diffuse reflection spectroscopy (DRS) technologies. Detailed physic-chemical measurements exhibited that all as-prepared nano-photocatalysts possesses both cubic (TbO1.81) and orthorhombic (TbCoO3) crystal structures. Furthermore, optical characterization by DRS developed light-sensitive channelization with band-gap energies at approximately 2.95 and 3.20 eV for Tb-Co-O nanocomposites. Finally, the photocatalytic studies of the resulting nanocomposites were compared by determining the elimination of Erythrosine (EY), Acid Violet 7 (AV7), and Acid Black 1(AB1) under UV and Visble light illumination. As a results, the TbCoO3/TbO1.81 nanocomposties with molar ratio of 1:3 (Tb:Co), valerian distillate as natural directing agent and ethylenediamine (en) as alkaline template yielded the optimum degradation percentage of 88 % for EY dye under the reaction condition of 10 ppm dye concentration in the presence UV light toward other pathways. Also, we proposed a mechanistic insight of photodegradation based on the radical scavengers, which revealed that h+ did the important role, and OH• and •O2− represented an irrelevant role in the degradation of EY. The current study offer an effective way for development of a high-efficiency Tb-Co-O photocatalyst in eliminating dyes from contaminant water.