Increasing demand for lithium-ion batteries (LIBs) that serve as power source for diverse electronic devices, electrical propulsion systems and other applications, calls for economical and environmentally benign recycling of spent LIBs and recovery of critical elements such as Co and Li from rapidly growing volumes of battery wastes. The presented study explores mechanochemical extraction of Co and Li from lithium cobaltate (LiCoO2), which serves as cathode material in commercial LIBs. Our investigation reveals that solvent-free mechanochemical processing can successfully convert pure, reagent grade LiCoO2 into metallic Co and Li-derivatives that are suitable for the further recovery of Li. We also show that the proposed approach can be successfully applied to reclaiming these critical elements from commercial LIBs. Due to its magnetic nature, metallic Co is easy to separate from non-magnetic components of mechanochemically generated powder mixtures using an appropriate magnetic separation technique, while Li can be reclaimed as Li2CO3 after an additional liquid-phase processing. The recovery rates achieved during our experiments with pure LiCoO2 are ∼90% for Co and ∼70% for Li.