A novel g-C3N4/α-Fe2O3–MoS2 (GFMO) ternary nanocomposite has been successfully constructed by facile calcination-hydrothermal methods. As-obtained magnetic GFMO ternary composite catalyst was investigated with the excellent degradation efficiency of organic rhodamine B (Rh B) and methylene blue (MB) pollutants in aqueous solution (95.6 % and 91.1 %) in 80 min under visible-light. The active coupling of α-Fe2O3 co-catalyst accelerated photo-electron transfer, improved visible-light fascination, suppressed the recombination rate, and sustained charge separation ability. This demonstrates the synergistic effect of the intimated heterojunction interface among g-C3N4 and MoS2, liable for efficient photo-degradation response. The scavenging tests revealed that •O2− and h+ reactive species play a most vital part in the photocatalytic degradation of both dyes. Furthermore, better electrocatalytic hydrogen evolution reaction (HER) performance in typical acidic conditions, with a lower overpotential of 305 mV and a Tafel slope of 128 mV dec−1. As an outcome, the current work offers a novel insight into the development of efficient ternary g–C3N4–based photocatalysts (PCs) for wastewater refining and electrochemical hydrogen evolution reactions.