Electrochemical impedance spectroscopy (EIS) was employed in an attempt to gain insight into the mechanisms of ethyl 2-cyanoacrylate (ECA) curing (polymerisation) and bonding on aluminium alloy 2024 metal. EIS can detect ionic movement, adsorption processes, charge transfer and storage occurring at an adhesive/substrate interface and/or in a bulk bond line during curing. Low-frequency capacitance measurements demonstrated sensitivity to surface polymerisation reactions and were modelled using an equivalent circuit model with two time constants in series. At a frequency of 1 kHz, changes in the dielectric polymer could be readily followed with time, confirmed by employing a crown ether to accelerate the polymerisation process. Hydrolytic degradation of poly-ECA bonds at a stainless steel interface was also investigated. An equivalent circuit model containing a number of circuit components comprising pore, charge transfer and diffusional impedances, along with polymer film, double layer and diffusional capacitances (represented by constant phase elements), was developed. Three regions were identified in the frequency domain and ascribed to processes taking place at the polymer/electrolyte and polymer/metal oxide interfaces. In short, EIS can be employed to follow the rate of polymerisation of ethyl-2-cyanoacrylate and also the degradation of the resulting polymer in saline solution.