The optimization of composite cure cycles is critical in materials engineering, requiring a deep understanding of the material’s cure kinetics. This study employs Differential Scanning Calorimetry (DSC) coupled with advanced fitting algorithms to determine the most accurate cure kinetics models for optimizing time-temperature profiles. Given the wide variability in model selection and fitting approaches in existing literature, our research systematically compares several cure kinetics models and their fitting methodologies to identify the most effective strategies. We highlight the advantages and limitations of each approach, with a particular focus on the robustness of the Levenberg–Marquardt (LM) algorithm compared to the Trust-Region-Reflective (TRR) algorithm. Given the existence of multiple local minima in the objective function, a global approach (genetic algorithm) is employed. Our findings reveal that, although the TRR and LM algorithms are faster, they are less accurate than the genetic algorithm. Moreover, the Kamal-Sourour model shows the highest prediction accuracy among the tested models. This comparative analysis provides a systematic approach and crucial insights into selecting the optimal cure kinetic model and corresponding parameters, based on experimental data, allowing for enhancing the efficiency and accuracy of composite curing processes.