This study was carried out to evaluate the efficiency and mechanism of P removal by different types of Fe-OM associations in peatlands. Humic substance (HS) and particulate organic matter (POM) were isolated from peat soils, and different types of iron-organic matter associations (Fe-HS and Fe-POM) were prepared. In addition, the natural combination of Fe3+ with peat was simulated. Then, isothermal adsorption experiments were carried out on the synthesized Fe-OM and iron-contained peat soils. All the adsorption data can be well fitted by the Langmuir adsorption model. The theoretical maximum adsorption capacity (Qmax) of Fe-HS associations can reach 36.90 mg/g, which is approximately two times higher than that of ferrihydrite (19.23 mg/g) and ten times higher than that of hematite (3.26 mg/g) and goethite (2.08 mg/g). The adsorption capacities of peat soils and POM were significantly enhanced by combinations with exogenous Fe3+. The Qmax of the original peat and iron-contained peat were 2.83 mg/g and 7.36 mg/g, respectively, and those of the original POM and Fe-POM association were 4.31 mg/g and 5.89 mg/g, respectively. The contribution of Fe-OM associations to phosphorus removal in peatlands is much higher than that of inorganic iron oxide. In addition, exogenous Fe3+ could also participate in other phosphorus removal processes.