Iron-modified corn straw biochar was used as an adsorbent to remove phosphorus from agricultural runoff. When agricultural runoffs with a total phosphorus (TP) concentration of 1.86 mg·L to 2.47 mg·L were filtered at a hydraulic retention time of 2 h through a filtration column packed with the modified biochar, a TP removal efficiency of over 99% and an effluent TP concentration of less than 0.02 mg·L were achieved. The isotherms of the phosphorus adsorption by the modified biochar fitted the Freundlich equation better than the Langmuir equation. The mechanism of the phosphorus adsorbed by the modified biochar was analyzed by using various technologies, i.e. scanning electron microscopy (SEM), X-ray diffraction (XRD) analysis, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). The results indicated that the surface of the modified biochar was covered by small iron granules, which were identified as Fe O . The results also showed that new iron oxides were formed on the surface of the modified biochar after the adsorption of phosphorus. Moreover, new bonds of Fe-O-P and P-C were found, which suggested that the new iron oxides tend to be Fe (PO ) (OH) . Aside from removing phosphorus, adding the modified biochar into soil also improved soil productivity. When the modified biochar-to-soil rate was 5%, the stem, root, and bean of broad bean plants demonstrated increased growth rates of 91%, 64%, and 165%, respectively.