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• Synthesis of new side-chain liquid crystalline copolymers containing polarisable groups. • Azobenzene groups confer light-responsive character to the electrolytes. • Electro-donating and electro-withdrawing groups tailor molecular structure. • High conductivity values are reached (10–2.9 S·cm−1) under anhydrous conditions. • Ion conductivity occurs through nematic and smectic phases, decoupled from the polymer backbone. We have prepared and characterised a series of side-chain liquid crystalline homopolymers and terpolymers containing different azobenzene derivatives (R AzB), sulfonic groups (2-acrylamido-2-methyl-1-propanesulfonic acid, AMPS), and methyl(methacrylate) groups (MMA), as monomeric units. We have evaluated the effect of different para-substitutes of 6-(4-azobenzene -4′-oxy)hexyl methacrylate, at the side chains, OCH 3 , NO 2 and H, on the phase behaviour and conductivity of the new polymers. The copolymers can form smectic and nematic phases, depending on their composition, and have light responsiveness, conferred by the azobenzene chromophores. The terpolymer with methoxy terminations, MeOAzB/AMPS/MMA, exhibits the highest conductivity values of the series (10−2/10−3 S·cm−1 range) through liquid crystalline phases and with signs of decoupling from polymeric segmental motions. These materials are promising candidates to develop new light-responsive polymeric electrolytes for electrochemical conversion devices in which ionic conductivity under anhydrous conditions can be controlled by their nanostructure. [ABSTRACT FROM AUTHOR]