Considerable efforts have been made to develop effective and sustainable catalysts, e.g., carbon-/biochar-based catalyst, for the decontamination of organic pollutants in water/wastewater. Most of the published studies evaluated the catalytic performance mainly upon degradation efficiency of parent compounds; however, comprehensive and field-relevant performance assessment is still in need. This review critically analysed the performance indicators for carbon-/biochar-based catalytic degradation from the perspectives of: (1) degradation of parent compounds, i.e., concentrations, kinetics, reactive oxidative species (ROS) analysis, and residual oxidant concentration; (2) formation of intermediates and by-products, i.e., intermediates analysis, evolution of inorganic ions, and total organic carbon (TOC); and (3) impact assessment of treated samples, i.e., toxicity evolution, disinfection effect, and biodegradability test. Five most frequently detected pharmaceuticals and personal care products (PPCPs) (sulfamethoxazole, carbamazepine, ibuprofen, diclofenac, and acetaminophen) were selected as a case study to articulate the performance indicators for a holistic evaluation of carbon-/biochar-based catalytic degradation. This review also encourages the development of alternative performance indicators to facilitate the rational design of catalysts in future studies.