The potential of electrodialysis to recycle spent lithium-ion batteries was assessed by investigating the recovery of lithium(I) from a synthetic solution representative of the aqueous effluent generated by shredding spent lithium-ion batteries underwater. Likewise, electrodialysis was tested for the selective recovery of lithium(I) towards cobalt(II), nickel(II) and manganese(II) from a synthetic solution representative of the leaching liquor of cathode materials. NMR spectroscopy showed that the implementation of electrodialysis to extract lithium from the aqueous effluent produced during battery shredding underwater should take into account the presence of HF generated by PF6− hydrolysis. In particular, it seems relevant to perform shredding under calcium chloride solution in order to precipitate fluoride and reduce HF generation. This work also showed that electrodialysis is an interesting technology for selectively recovering lithium from the leach solution of spent cathode materials, providing that divalent cations were previously removed to avoid metal precipitation inside the electrodialysis membranes. After removing cobalt(II) and nickel(II) at pH 2.8 and manganese(II) partially at pH 5.5 by using the ion exchange resin Dowex M4195, it is possible to extract and selectively concentrate lithium by electrodialysis without coextracting manganese(II) by using a lithium-selective membrane (faradic efficiency of 57.6%, permselectivity for lithium towards manganese of 6.9). Finally, a hybrid flowsheet implementing mineral processing and hydrometallurgy, including electrodialysis, ion exchange and crystallization stages, was proposed based on these results to reduce effluent generation and produce metal salts from spent lithium-ion battery.