A technique has been developed based on Fourier transform infrared spectroscopy (FTIR) in the attenuated total reflectance (ATR) mode, which is suitable for the investigation of the heterogeneous cure of surface-initiated redox polymerizations in thin and thick bondline situations. The results of the investigations into the surface-catalyzed and anaerobically promoted cure of some model adhesives using this method are reported. The systems under investigation were designed to exhibit different levels of cure heterogeneity or "cure through volume" (CTV) so that the influence of the bondline thickness and the formulation variables may be assessed. The analysis of the data provides evidence that supports our concept of the heterogeneous cure distribution existing in the form of a cure gradient. This concept of a cure gradient is developed further using dielectric spectroscopy. Here the cure gradient is characterized in terms of the parameters obtained using an empirical equation to fit the dielectric relaxation data. The results obtained using the infrared and dielectric spectroscopic methods are in satisfactory agreement and are shown to be most informative in characterizing and quantifying the CTV performance of the model anaerobic adhesives.