In Fe2+/peroxymonosulfate (PMS) activation system, the slow cycle rate of Fe3+/Fe2+ has been considered to be the limiting step in the remediation of organic contaminants. In this paper, commercial molybdenum (Mo) powder is employed as the cocatalyst in Fe2+/PMS system, which can significantly accelerate the Fe3+/Fe2+ cycling efficiency by the exposed bimetallic active sites of Mo4+ and Mo0, and the process is accelerated as the amount of Mo powder increased. The Mo cocatalytic Fe2+/PMS system exhibits an enhanced performance for the activation of PMS and the removal of different aromatic pollutants including dyes, phenolic pollutants and antibiotics, in a wide pH range of 4.0-9.0. Importantly, Mo powder exhibits excellent cycle performance in the PMS activation system, and rhodamine B (RhB) can be removed within 10min even after 5 cycles. Electron paramagnetic resonance (EPR) prove that the sulfate radicals (SO4-) is the major reactive oxides species in the PMS activation, the increase of Fe2+ content induced by the cocatalytic effect of Mo powder can effectively promote the production of SO4- and increase the utilization of PMS. In addition, to observe the process of pollutant removal more intuitively, HPLC-MS is used to analyze the decomposing pathway of RhB and sulfadiazine in Mo+FeSO4+PMS system. It is believed that this research provides a new idea for the efficient activation of PMS by iron ions in a wide initial pH range, which is expected to be applied to the treatment of large-scale industrial wastewater.