We have successfully stabilized Cr leaching in Ti/Cr/Si ternary composites by adopting the Flame Spray Pyrolysis (FSP) synthesis technique and achieving higher photocatalytic activity in the visible light region. Initially, we have prepared a series of catalysts with different Si/Ti atomic ratios (80, 75, 70, 60, and 50) as well as (Si+Ti)/Cr ratios (8, 10, 15, 20, 25, and 30) and investigated their visible light photocatalytic activity. The effect of the Si and Cr atoms on the structural, optical, and photocatalytic properties of TiO2 has been investigated. Our XRD studies reveal that the (Si+Ti)/Cr ratios and Si/Ti atomic ratios alter the TiO2 lattice structure, with an increase in the Si ratio in the catalyst reduction of the rutile phase being observed. An increase in the Si/Ti atomic ratio from 50 to 75 monotonically transformed the rutile phase into the anatase phase. Introduction of Cr induced a substantial amount of disorder into the TiO2 lattice and altered the crystallinity. A high amount of Cr in the catalyst led to the transition from the tetrahedral coordination of CrO3 to the hexagonal coordination of Cr2O3 oxide and implies the segregation of chromium out of the TiO2 lattice. Dropping the Cr amount (an increase in the (Si +Ti)/Cr atomic ratio) to within solubility limits would solve the difficulties accompanying Cr2O3 segregation out of TiO2. The addition of SiO2 into the titania lattice greatly promoted the surface texture by enhancing the surface area by four times the commercial TiO2. The introduction of Cr extended the visible light absorption of the catalyst to 550 nm. Our H-2-TPR results suggest that the increase in the Si/Ti atomic ratio greatly promoted the suppression of the Cr2O3 phase in the catalyst along with an increase in reduction potential of Cr6+. It is found in our studies that Cr has an imperative role in the photocatalytic activity, while the SiO2 was found to be responsible for the stability of the photocatalyst. We have observed that the optimal flame-made Cr/Ti/Si catalyst demonstrated an extremely low level of Cr and Ti leaching throughout the photocatalytic degradation reaction, therefore inhibiting the contamination of the treated wastewater due to secondary metal leaching. We observed a stable Cr(IV) concentration for the reused catalyst, which plays an important role in improved and stable photocatalytic activity in the visible region for the materials. Unlike the Cr/TiO2 systems, the optimal flame-made Cr/Ti/Si catalyst established high efficiency in visible photocatalysis, stability, and reusability without any Cr leaching even after five consecutive cycles.