hazardous substances. Among the popular AOPs, the homogeneous and heterogeneous Fenton reactions are most promising with their preponderance in the vast application range, strong anti-interference ability, simple operation, and rapid degradation speeds. [1,2] However, three main limitations still challenge the practical application of the classic homogeneous Fenton process using iron or copper ions, including the slow-cycling efficiency of Fe 3+ /Fe 2+ or Cu 2+ /Cu + , accumulation of iron/copper-containing sludge, and strict requirement of low pH (3.0-4.0). [3,4] Researchers have gradually turned to heterogeneous Fenton-like catalysis to avoid the generation of ferric hydroxide sludge and circumvent the limitation of the acidic pH range on homogeneous Fenton reactions. [5] To address the aforementioned issues, strenuous efforts have been devoted to designing Fe or Cu species in solid catalysts. They are usually given priority in superior heterogeneous Fenton catalysts because of the low cost, negligible toxicity, high catalytic activity, and ease of recovery. [6] Therefore, combining Fenton-like systems with photocatalysts has attracted intensive research interest with their rapid development.Graphitic carbon nitride (g-CN)-supported Fe, Cu catalysts are well recognized as good choices for heterogeneous photo-Fenton catalysts. As the host, g-CN serves as a visible-lightactive metal-free polymeric semiconductor with an appropriate band gap (≈2.7 eV) to harvest solar photon energy efficiently. [7] It can also be employed to construct various highly tailorable composite photocatalysts with adjustable compositions, sizes, pore structures, morphology, and electronic structures. [8][9][10] g-CN can be loaded with Fe or Cu atoms and nanoparticles to form high-performance Fe-CN or Cu-CN photo-Fenton systems, which further accelerates the rate-limiting Fe 3+ /Fe 2+ or Cu 2+ /Cu + reduction process and circulation of high-valence metal ions in the presence of light, thus avoiding the generation of hazardous iron or copper sludge.Up to now, the efficiency of photo-Fenton systems is still unsatisfactory for industrial applications. To further improve the efficiency of heterogeneous Fenton-like reactions, much effort has been carried out to optimize AOPs, including the strategy of adding co-catalysts to boost •OH or singlet oxygen Heterogeneous Fenton-like process with a wide pH range is a promising alternative to traditional homogeneous Fenton reactions. Recently, the boosting effect of MoS 2 cocatalysts is widely recognized in Fenton reactions, and the primary mechanism is the promotion of the reduction and recycling of high-valence metal ions. Unfortunately, integrating heterogeneous Fenton-like catalysts and MoS 2 cocatalyst to form an efficient system remains challenging due to the severe deactivation of MoS 2 and the inability of simple physical mixing to speed up the reaction. For the first time, the direct activation of commercially available bulk MoS 2 powder in a durable acidic micro environment is achieved. The fo...