Structural electrolytes' retain the desirable mechanical characteristics of structural (epoxy) resins whilst introducing sufficient ionic conductivity to operate as electrolytes in electrochemical devices. Here, a series of ionic liquid-epoxy resin composites were prepared to identify the optimum system microstructure required to achieve a high level of multifunctionality. The ionic conductivity, mechanical properties, thermal stability and morphology of the cured epoxy based structural electrolytes were studied as a function of phase composition for three fully formulated high performance structural epoxy systems. At only 30 wt% of structural resin and 70 wt% of ionic liquid based electrolyte, stiff monolithic plaques with thicknesses of 2-3 mm were obtained with a room temperature ionic conductivity of 0.8 mS cm À1 and a Young's modulus of 0.2 GPa. This promising performance can be attributed to a long characteristic length scale spinodal microstructure, suggesting routes to further optimisation in the future.