Fiber-reinforced polymer (FRP) structures and components are highly susceptible to damage due to delamination, matrix cracking, inter-laminar fracture, and debonding, all of which have potential to cause catastrophic structural failure. While numerous sensing technologies have been developed and embedded in FRP composites for monitoring strain, they serve as defects and can promote damage formation and propagation. Thus, in this study, an alternative technique is proposed for in situ strain monitoring of FRP composites via layer-by-layer multi-walled carbon nanotube-polyelectrolyte thin films deposited directly upon glass fiber weaves. To date, these carbon nanotube-based thin films have been validated for their piezoresistivity. The objective of this study is to characterize the strain sensing performance of different thickness thin films deposited on glass fiber weaves and embedded in FRP specimens using time-domain two-point probe resistance and frequency-domain electrical impedance spectroscopy (EIS) measurements. From the experimental thin film electromechanical response, a new method for fitting using a cubic smoothing spline is implemented and is compared to linear least-squares fitting. The results show that the cubic spline fit is better suited for capturing the strain sensitivities (or gage factors) of these thin films within the time- and frequency-domains along with the variation of strain sensitivity with applied strain. The bulk resistance response is described by the DC resistance measurements, whereas the EIS measurements provide insight of the inter-nanotube response.