This research mainly focused on the phosphorus removal performance of pilot-scale vertical flow constructed wetlands with steel slag (SS) and modified steel slag (MSS). First, bench-scale experiments were conducted to evaluate the phosphorus adsorption capacity. Results showed that the Langmuir model could better describe the adsorption characteristics of the two materials; the maximum adsorption of MSS reached 12.7 mg/g, increasing by 34% compared to SS (9.5 mg/g). Moreover, pilot-scale constructed wetlands with SS and MSS were set up outdoors. Then, the influence of hydraulic retention time (HRT) and phosphorus concentration in phosphorus removal for two wetlands were investigated. Results revealed that better performance of the two systems could be achieved with an HRT of 2 d and phosphorus concentration in the range of 3–4.5 mg/L; the system with MSS had a better removal efficiency than the one with SS in the same control operation. Finally, the study implied that MSS could be used as a promising substrate for wetlands to treat wastewater with a high phosphorus concentration. However, considering energy consumption, SS could be regarded as a better alternative for substrate when treating sewage with a low phosphorus concentration.