A novel Fe/amine modified chitosan composite (Fe/N-CS) was facilely synthesized and showed higher affinity to both Zn(Ⅱ) and cefazolin (CEF) than its precursors. Synergistic co-adsorption of them by Fe/N-CS was observed in varied conditions. The adsorption amount maximally increased by 100.1% for Zn and 68.2% for CEF in bi-solute systems. The initial adsorption rate of Zn(Ⅱ) also improved with CEF. The increasing temperature facilitated coadsorption. The results of the preloading tests, FTIR/XPS characterizations and DFT calculations suggested that (1) both polyamines and Fe sites participated in the adsorption of Zn(Ⅱ) and CEF, (2) Zn(Ⅱ) could serve as a new efficient site for CEF, forming [amine-Zn-CEF]/[FeOH-Zn-CEF] tary complexes, and (3) the co-presence of CEF shielded the electrostatic repulsion between protonated amines and Zn(Ⅱ), contributing to the enhancement of Zn(Ⅱ) adsorption. Further, the ion strength exerted positive and negative influences on the adsorption of Zn(Ⅱ) and CEF, respectively. Additionally, CEF and Zn(Ⅱ) were successively recovered by 0.1 mol/L NaOH followed by 2 mmol/L HCl. Fe/N-CS could be stably reused five times. The findings imply that Fe/N-CS is promising for the highly efficient co-removal of concurrent heavy metals and antibiotics.