Graphene aerogel with well-distributed CoO nanoparticles (CoO@GA) has been subtly fabricated by using methylamine as a multifunctional agent through hydrothermal and calcination processes for the degradation of chloramphenicol (CAP). The results showed that CoO@GA containing 27.3 wt% of CoO nanoparticles with size ranging from 30 to 60 nm exhibited high mechanical elastic property. The cyclic compression testing with strain up 50% showed CoO@GA can completely recover to its original form after compression. Compared with bare CoO, Co2+ or GA, CoO@GA performed the best degradation efficiency for CAP (95.8%) in the presence of peroxymonosulfate (PMS). Quenching experiment indicated HO and O2- were the main active radicals generated in the CoO@GA-PMS system. The recycled experiments showed CoO@GA had stable efficiency (above 82.8%) within 9 times for the degradation of CAP.