Atomic-scale integration of polyether molecules and copper(II) chloride layers in a two-dimensional perovskite affords, to the best of our knowledge, the first example of extended Li+ cycling in a metal chloride electrode. The hybrid can cycle over 200 times as a cathode in a lithium battery with an open-circuit voltage of 3.2 V. In contrast, CuCl2 alone or the precursors to the hybrid cannot be cycled in a lithium battery, demonstrating the importance of the layered, organic inorganic architecture. This work shows that appropriate organic groups can enable Li+ cycling in inexpensive, nontoxic, metal halide electrodes, which is promising for large-scale applications.