Display omitted •Ultrafine magnetic carbonaceous sorbents are successfully prepared by ball milling.•Biochar/Fe3O4 exhibits fast and high sorption for carbamazepine and tetracycline.•Ultrafine biochar/Fe3O4 and AC/Fe3O4 can be separated magnetically.•Ball milling is effective for degradation of adsorbed CBZ/TC on the adsorbents.•Addition of quartz sand improves the mechanochemical degradation of CBZ. Ball milling was used to prepare two ultrafine magnetic biochar/Fe3O4 and activated carbon (AC)/Fe3O4 hybrid materials targeted for use in pharmaceutical removal by adsorption and mechanochemical degradation of pharmaceutical compounds. Both hybrid adsorbents prepared after 2h milling exhibited high removal of carbamazepine (CBZ), and were easily separated magnetically. These adsorbents exhibited fast adsorption of CBZ and tetracycline (TC) in the initial 1h. The biochar/Fe3O4 had a maximum adsorption capacity of 62.7mg/g for CBZ and 94.2mg/g for TC, while values obtained for AC/Fe3O4 were 135.1mg/g for CBZ and 45.3mg/g for TC respectively when data were fitted using the Langmuir expression. Solution pH values slightly affected the sorption of TC on the adsorbents, while CBZ sorption was almost pH-independent. The spent adsorbents with adsorbed CBZ and TC were milled to degrade the adsorbed pollutants. The adsorbed TC itself was over 97% degraded after 3h of milling, while about half of adsorbed CBZ were remained. The addition of quartz sand was found to improve the mechanochemical degradation of CBZ on biochar/Fe3O4, and its degradation percent was up to 98.4% at the dose of 0.3g quarts sand/g adsorbent. This research provided an easy method to prepare ultrafine magnetic adsorbents for the effective removal of typical pharmaceuticals from water or wastewater and degrade them using ball milling.