(T)his paper focuses on the in situ characterization of methylsilsesquioxane curing. As the final properties of this material depend on the curing process, it is important to investigate the mechanisms operating during its cross-linking process. Thermal analysis techniques such as dielectric analysis, differential scanning calorimetry, thermomechanical analysis, and thermogravimetric analysis are employed to carry out an in-depth study on its curing. The curing of methylsilsesquioxane is found to be an endothermic process accompanied by weight loss, shrinkage and reduction in coefficients of thermal expansion and dielectric constant. A two-stage curing process has also been postulated based on the data collected. The dielectric analyzer provides real-time molecular relaxation of the dielectric material before, during, and after the curing process.