In this paper, groundwater treatment sludge (GTS) was recycled as a magnetic adsorbent via a facile calcination process without adding any reductant. The prepared magnetic adsorbents (MAs) were characterized by scanning electron microscopy (SEM), X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS), vibrating sample magnenometer (VSM) and Mössbauer spectroscopy. The results showed that GTS comprised 33.2% Fe, 1.4% Al and 6.2% Si, and exhibited a weak saturation magnetization of 0.0008 emu/g. Without NaOH, the GTS calcinated at 700 and 500 °C were well magnetized with Ms of 20.1 and 7.1 emu/g, separately, but exhibited a low Ms of 0.43 emu/g at 300 °C. By adding NaOH powder, the Ms of GTS apparently increased to 4.9 emu/g after calcination at 300 °C, and further to 8.5 emu/g at 500 °C. In GTS, about 96.1% Fe was involved in ferrihydrite form. The Ms of calcinated GTS was accompanied with the phase transformation of ferrihydrite to maghemite. Si/Al oxides in GTS coordinated on the surface sites of ferrihydrite and inhibited the conjunction and phase transformation of adjacent ferrihydrite particles, but were effectively desorbed as in the presence of NaOH. Na500, preparing by calcinating GTS at 500 °C with NaOH, showed an optimal total surface sites (Hs) of 0.65 mmol/g. Oxytetracycline (OTC) was used as a target for studying the adsorption characteristics of synthetic magnetic adsorbents and a high adsorption capacity of oxytetracycline of 862.1 mg/g in comparison with the other calcinated GTS, and the adsorption data was consistent with the Langmuir model. By adding 6 g/L Na-500, approximately 100% of oxytetracycline and tetracycline and nearly 40% total organic carbon were removed from real pharmaceutical wastewater. With the method, GTS can be converted in mass production to magnetic adsorbent that exhibits effective application in pharmaceutical wastewater treatment.