A lot of attention has been drawn to photo-Fenton-like catalysis among advanced oxidation processes for environmental remediation applications. Herein, we have successfully fabricated iron-nickel bimetallic magnetic nano-alloy (INBMNA) as an efficient heterogeneous photo-Fenton-like catalyst using the chemical reduction method and characterized by several analytical techniques. The characterization results show that the catalyst has a spherical shape with a mesoporous nature and contains a large specific surface area. The impact of various parameters was investigated and optimized to check the catalytic performance of INBMNAs and the found results showed that excellent photo-Fenton-like activity persisted under 6.0 pH conditions for the degradation of hazardous pollutant (phenol) under solar light exposure and microwave radiation power, respectively. Additionally, the exposed INBMNA/H2O2 system provided continuous redox cycles of Fe3+/Fe2+ and Ni2+/Ni0 pair in the Fenton-active species for stable operation. The photo-Fenton-like activity was also performed to check the effect of different inorganic anions which significantly hinder phenol reduction. Besides, the steady performance of the catalyst to remove phenol was performed in tap water and river water. Free radical trapping experiments were tested to know the role of important radicals in the photo-Fenton process. Moreover, the mechanism and possible degradation pathways of phenol were checked. By cyclic degradation experiments, the performance of the catalyst is stable and almost unchanged and can be reused several times. This study provides a promising INBMNA/H2O2 system, which encourages its widespread use in environmental remediation applications.