The development of effective approaches for the preparation of 0D quantum dots (QDs)/2D nanosheets (NSs) heterostructures, which have been proven to be favorable for heterogeneous catalysis, is highly desirable but remains a great challenge. Herein, 0D metal oxide nanocrystals-2D ultrathin g-C N nanosheets (Co O /CNNS) heterostructures are synthesized via a facile chemical reaction, followed by annealing in air. Ultrafine Co O QDs (≈2.2-3.2 nm) are uniformly and tightly attached on the surface of g-C N nanosheets. Detailed characterization reveals that the specially designed unique 0D/2D structure is critical to the high photocatalytic performance for the degradation of tetracycline (TC) via peroxymonosulfate (PMS) activation. The optimal catalyst, namely, Co O /CNNS-1100, exhibits excellent performance and ≈98.7% TC can be degraded under visible light irradiation. Moreover, TC degradation is almost completely insusceptible to several real water samples. Meanwhile, other dye pollutants can also be efficiently degraded by the Co O /CNNS-1100/PMS/vis system. The quenching tests display that that the h , ∙OH, O , and SO are responsible for TC removal. The improved photocatalytic performance can be attributed to the synergistic effect of the photocatalytic- and chemical-processes in the PMS activation. This work gives an insight into the development of multifunctional 0D/2D nanocomposites for further potential applications which are not limited to environmental purification.