Cobalt　spinel　oxide　(Co3O4)　is　a　promising　nonprecious　catalyst　for　methane　combustion,　and　improving　its　catalytic　performance　through　structural　modulation　is　desirable.　Herein,　layer-structured　Cu2+-Co2+-Co3+　hydrotalcite-like　compounds　(HTlcs)　were　synthesized　via　methanol-assisted　oxidative　intercalation　and　used　as　a　single-source　precursor　to　prepare　copper-cobalt　spinels　for　the　first　time.　Their　characterizations　reveal　that　single-phase　and　composition-tunable　Cu2+-Co2+-Co3+　HTlcs　are　quantitatively　formed.　Upon　calcination,　Cu-Co　HTlcs　are　decomposed　into　CuxCo3-xO4　spinels　with　a　copper　content　of　up　to　10　at.%.　X-ray　photoelectron　spectroscopy　and　X-ray　absorption　spectroscopy　indicate　that　copper　ions　are　incorporated　into　the　Co3O4　lattice　as　tetrahedrally　coordinated　Cu+/Cu2+　and　octahedrally　coordinated　Cu2+.　The　presence　of　abundant　Cu+　suggests　a　redox　cycle　between　Co3+/Co2+　and　Cu2+/Cu+　couples,　highlighting　a　strong　electronic　interaction　between　copper　and　cobalt　species.　The　strong　Cu-O-Co　interaction　not　only　increases　oxygen　vacancies　and　surface　lattice　oxygen　mobility　by　weakening　the　Co-O　coordination　but　also　drastically　enhances　cobalt　reducibility.　Copper-cobalt　spinels　exhibit　noticeably　improved　catalytic　activity,　and　the　highest　activity　is　observed　for　Cu10-Co3O4,　facilitating　nearly　complete　CH4　conversion　at　500　degrees　C　under　a　space　velocity　of　36,000　mL　gcat　-　1h-　1.　This　catalyst　also　manifests　good　cycle　stability,　long-term　stability,　and　resistance　to　water　vapor.　The　synergetic　effect　between　Co3+/Co2+　and　Cu2+/Cu+　redox　couples　plays　a　key　role　in　improving　catalytic　activity.　The　proposed　HTlc　strategy　may　provide　a　new　opportunity　for　the　controlled　preparation　of　various　bimetallic　and　multimetallic　cobaltite　spinels　for　different　applications.