In this paper, coconut shell biochar (BC), pickling biochar (HBC), and nano-zero-valent iron-loaded biochar (nZVI-HBC) were prepared; these were used to remove oxytetracycline (OTC), and the removal mechanism and degradation product were analyzed. These biochars were characterized using SEM, XRD, FTIR, and XPS. The effects of biochar addition amount, pH, ion type, and ion concentration on OTC adsorption were studied by a batch adsorption experiment. Under the optimal conditions, the equilibrium adsorption capacity of nZVI-HBC to OTC was 196.70 mg·g−1. The adsorption process can be described by Langmuir isothermal adsorption equations, conforming to the pseudo-second-order dynamics model, indicating that adsorption is dominated by single-molecule chemical adsorption, and a spontaneous process of increasing heat absorption entropy. Mass spectrometry showed that the OTC removal process of nZVI-HBC included not only adsorption but also degradation. These results provide a practical and potentially valuable material for the removal of OTC.