Abstract In this work, we developed a facile method for photocatalytic deposition of cobalt atoms as co-catalyst on TiO2 nanosheets (Co(x)/T) under visible light instead of UV irradiation for the first time. The deposition of cobalt atoms on TNs in the Co(x)/T samples was confirmed by DRS, Raman spectroscopy, photoluminescence, nitrogen physisorption, and TEM analyses. The size of cobalt nanoparticles/cluster dispersed on the TiO2 nanosheets were in the range of 5–20 nm according to TEM results. The PXRD patterns showed that the crystal structure and the anatase phase of TNs were preserved in the Co(x)/T samples after the visible light-assisted deposition process. The Co(x)/T samples showed higher activity compared to pure TiO2 nanosheets for the visible light degradation of tetracycline (TC) as pharmaceutical pollutant due to presence of cobalt co-catalyst. We studied the effect of several parameters on the degradation process and proposed the mechanism of degradation according to quenching experiments results. Due to time-consuming and costly of experimental works, we designed two strong artificial intelligence (AI) models (artificial neural networks (ANN) and neuro-fuzzy inference systems (ANFIS)) to estimate the removal process of TC, and predict the removal percent of TC for new values of inputs before performing experiment. The experimental and computational studies showed that the fabricated photocatalysts are as promising candidates for industrial wastewater treatment to meet environmental regulations and provide a new avenue for practical implications.