To elucidate the adsorption property and the mechanism of plant residues to reduce oxytetracycline (OTC), the adsorption of OTC onto raw willow roots (WR-R), stems (WS-R), leaves (WL-R), and adsorption onto desugared willow roots (WR-D), stems (WS-D), and leaves (WL-D) were investigated. The structural characterization was analyzed by scanning electron microscopy, Fourier-transform infrared spectra, and an elemental analyzer. OTC adsorption onto the different tissues of willow residues was compared and correlated with their structures. The adsorption kinetics of OTC onto willow residues was found to follow the pseudo-first-order model. The isothermal adsorption process of OTC onto the different tissues of willow residues followed the Langmuir and Freundlich model and the process was also a spontaneous endothermic reaction, which was mainly physical adsorption. After the willow residues were desugared, the polarity decreased and the aromaticity increased, which explained why the adsorption amounts of the desugared willow residues were higher than those of the unmodified residues. These observations suggest that the raw and modified willow residues have great potential as adsorbents to remove organic pollutants.