This paper focuses on monitoring of carbon nanotube (CNT) network development during the cure of unsaturated polyester nanocomposites by means of electrical impedance spectroscopy. A phenomenological model of the dielectric response is developed using equivalent circuit analysis. The model comprises two parallel RC elements connected in series, each of them giving rise to a semicircular arc in impedance complex plane plots. An established inverse modelling methodology is utilized for the estimation of the parameters of the corresponding equivalent circuit. This allows a quantification of the evolution of two separate processes corresponding to the two parallel RC elements. The high frequency process, which is attributed to CNT aggregates, shows a monotonic decrease in characteristic time during the cure. In contrast, the low frequency process, which corresponds to inter-aggregate phenomena, shows a more complex behaviour explained by the interplay between conductive network development and the cross-linking of the polymer.