To improve the photocatalytic performance of TiO2 photocatalysts, a new method, liquid phase plasma (LPP) method, was used to introduce nitrogen and iron oxide. Interstitial or substitutional nitrogen and Fe3+ iron nanoparticles were impregnated on the surface of TiO2 by LPP reaction without additional chemical reduction agent and the amount of iron of modified TiO2 photocatalysts was affected by the amount of initial precursor. The adsorption edge of modified TiO2 photocatalysts was shifted to the visible region in proportion to the amount of nitrogen and iron oxide, and the band gap energy was decreased, and the photocatalytic activity was confirmed by PL and EPA analysis. The photocatalytic activities of modified TiO2 photocatalysts were measured under UV and blue LED lamps and compared with pure TiO2 powder (P-25). The modified TiO2 exhibited better photocatalytic degradation performance than pure TiO2 under blue LED light conditions, but exhibited low degradation activity under UV LED light conditions. Through GC-MS analysis, it was found that the methylene blue was finally decomposed into an inorganic substance through intermediates such as benzene sulfonic acid and phenol by OH radicals. From these results, we found that the modified TiO2 photocatalysts can be easily prepared using the LPP method and can be used in the visible region.