In this work, we are focusing on the production of LiOH from Li2SO4 electrodialysis as it is the common product from hardrock-mining leaches after the acid-roasting of the spodumene mineral with sulphuric acid. To rationalise, understand and target the optimal membrane compositions for their application as CEMs for producing LiOH by Li2SO4 electrodialysis, new copolymeric membranes were synthesised based on different combinations of methacrylic co-monomers with different degrees of crosslinking.