In this study, crayfish shell biochar (CSB) was modified by introducing vitamin C (VC) with abundant surface functional groups. CSB was impregnated with VC at different ratios and its capacity to adsorb tetracycline (TC) from water was analyzed. The physicochemical properties of CSB were determined by N2 adsorption-desorption isotherm analysis, X-ray diffraction, and Fourier transform infrared spectroscopy. The effects of various factors on adsorption such as the pH, TC concentration, time, and salt ion concentrations were also investigated. Based on the chemical structure of VC, VC can provide CSB with more oxygen-containing functional groups such as hydroxyl groups. The results showed that the CSB modified with VC (CSB-VC) exhibited excellent adsorption of TC, and CSB-VC2 with an impregnation ratio of 2 (gVC/gCSB) had the greatest adsorption performance (saturated adsorption capacity, Qm = 293.36 mg/g), whereas the adsorption performance of CSB alone was about 50% lower (Qm = 172.16 mg/g). The optimal impregnation ratio VC improved the adsorption performance of CSB after modification to 70.4% of the original. Hydrogen bonding, p-p conjugation, pi-pi electron donor-acceptor effect, and π-π interactions were identified as the main adsorption mechanisms. CSB-VC2 was highly effective over a wide range of pH values and at high ion concentrations. Experiments demonstrated the effective regeneration of the adsorbent after multiple cycles, thereby indicating its excellent reusability. It should be noted that the adsorption capacity was good under different water quality conditions, and thus it should exhibit stable adsorption performance under complex water environment conditions.