Azo dyes make up a major class of dyes that have been widely studied for their diverse applications. In this study, we successfully applied nano-γ-Fe 2 O 3 /TiO 2 as a nanocatalyst to improve the photodegradation efficiency of azo dyes (Orange G (OG) dye as a model) from aqueous solution under white lightemitting diode (LED) irradiation. We also investigated the degradation mechanisms and pathways of OG dye as well as the effects of the initial pH value, amount of H 2 O 2 , catalyst dosage, and dye concentration on the degradation processes. The characterizations of nano-γ-Fe 2 O 3 and γ-Fe 2 O 3 Nps/TiO 2 were carried out using various techniques, including X-ray diffractometry, scanning electron microscopy, energy-dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, and UV− visible spectroscopy. The efficiency of the photodegradation reaction of OG was found to follow pseudo-first-order kinetics (Langmuir−Hinshelwood model) with a rate constant of 0.0338 min −1 and an R 2 of 0.9906. Scavenger experiments revealed that hydroxyl radicals and superoxide anion radicals were the dominant species in the OG photocatalytic oxidation mechanism. This work provides a new method for designing highly efficient heterostructure-based photocatalysts (γ-Fe 2 O 3 Nps/TiO 2 ) based on LED light irradiation for environmental applications.