Organic pollutants (OPs) are potentially present in composts, and the assessment of their content and bioaccessibility in these composts is of paramount importance to minimize the risk of soil contamination and improve soil fertility. In this work, integration of the dynamics of organic carbon (OC) and OPs in an overall experimental framework is first proposed and adopted to validate the applicability of the COP-Compost model and to calibrate the model parameters on the basis of what has been achieved with the COP-Compost model. The COP-Compost model was evaluated via composting experiments containing 16 US Environmental Protection Agency (USEPA) polycyclic aromatic hydrocarbons (PAHs) and the sorption coefficient (Kd) values of two types of OP: fluorenthene (FLT) and pyrene (PHE). In our study, these compounds are used to characterize the sequential extraction and are quantified as soluble, sorbed, and non-extractable fractions. The model was calibrated, and coupling the OC and OP modules improved the simulation of the OP behavior and bioaccessibility during composting. The results show good agreement between the simulated and experimental results describing the evolution of different organic pollutants using the OP module, as well as the coupling module. However, no clear relationship is found between the Kd and the property of organic fractions. Further estimation of parameters is still necessary to modify the insufficiency of this present research.