A novel method for in situ synthesis of Fe, N, Co tri-TiO₂ (DT) loading on MCM-41 composite photocatalyst was proposed. Fe, N, Co tri-TiO₂@MCM-41 (DTM) with adsorption-degradation synergy was prepared by adjusting tetrabutyl titanate (TBOT) concentrations, the alcohol-water ratio in the atmosphere of the reaction chamber. The influence of preparation parameters on the texture structure, catalytic activity, and the synergism of adsorption and degradation of the DTM was discussed, the optimal parameters were determined. The DTM was characterized by XRD, TEM, BET, FT-IR, and UV-Vis. Besides, the DTM exhibited obvious redshift and visible catalytic activity compared with undoped TiO₂@MCM-41 (TM), which possessed excellent performance in the degradation of gaseous and liquid pollutants. The degradation rate of methylene blue (MB) and nitric oxide (NO) was 96.39% and 56.75%, respectively. Furthermore, DTM photocatalyst exhibited excellent reusability. The degradation efficiency of MB and NO after five cycles decreased by 4.54% and 5.89%, respectively.