Highly robust ceramics materials are promising materials for applications in the automobile, aerospace, and ceramic cutting tool industries. However, conventional ceramics are typically brittle, which limits their suitability for advanced applications. In this study, with zeolite imidazolium salt skeleton-8 (ZIF-8) as a carbon source, discharge plasma sintering is used to create carbon nanonetworks derived from metal-organic frameworks (MOFs) in situ on the grain boundaries of zirconia-toughened alumina (ZTA) ceramic. ZTA exhibits maximum bending strength (719 ± 20.5 MPa) and fracture toughness (7.91 ± 0.7 MPa m1/2) at MOF concentrations of 1.0 wt% and 2.0 wt%, respectively, which are 1.37 and 1.88 times higher than that of the unmodified sample. This demonstrates that the MOF-derived carbon nanonetworks significantly improve the mechanical properties of the ceramic. The finite element analysis results indicate that the carbon nanonetworks can effectively disperse the stress inside the material and transfer the concentrated stress from the internal defects to the two-phase grain boundary on the surface of the sample, thereby contributing to strengthening and toughening. Overall, this work validates that the in situ production of carbon nanonetworks from MOFs is an effective strategy to enhance the mechanical properties of ZTA ceramics. Moreover, it offers new approaches for reinforcing and toughening other ceramic materials.