In recent years, the development of environmentally friendly solid catalysts derived from sludge for the efficient removal of pollutants from wastewater has triggered widespread attention. Acid mine drainage (AMD) sludge is a waste produced in the process of acid mine wastewater treatment and contains multitudes of valuable metal resources. Hence it provides the original conditions for the synthesis of metal-based Fenton catalysts. In this article, the Fenton-like catalyst Al-Fe3O4 derived from AMD sludge was first synthesized by acid leaching coprecipitation methods, and the relationship among catalyst properties and pH, growth temperature, and growth time during coprecipitation was explored. Transmission electron microscope (TEM)/vibrating sample magnetometer (VSM)/particulate size description analyzer (DLS) results showed that the Al-Fe3O4 catalyst with high purity, large particle size, and strong magnetic properties was obtained under the conditions of pH 10, reaction temperature 60 °C, and growth for 45 min. In addition, the introduction of Al active sites promoted the activation of H2O2 and improved the catalytic activity of Al-Fe3O4, and the degradation efficiency of tetracycline was up to 93.9% within 60 min, which was 1.94 times that of pure Fe3O4. Moreover, Al-Fe3O4 exhibited excellent recyclability after four adsorption-desorption cycles. Hence, this study is expected to promote the resource utilization of industrial sludge and provide a new idea for the rapid removal of TC from aqueous solution.