The　hydration　of　calcium　aluminate　cement　(CAC)　generates　metastable　phases　such　as　CAH10　and　C2AH8,　which　subsequently　transform　into　more　stable　products,　leading　to　a　reduction　in　strength　and　causing　volumetric　instability.　The　present　study　aims　to　alter　the　hydration　pathway　with　improved　mechanical　strength　and　volume　stability　of　CAC　by　carbonation　curing　with　different　temperatures　and　durations.　The　mechanical　strength,　dimensional　changes,　carbonation　products,　and　microstructure　were　comprehensively　investigated.　The　results　reveal　that　carbonation　curing　converts　the　metastable　hydration　products　C2AH8　and　CAH10　of　CAC　directly　into　AH3　and　calcium　carbonate,　primarily　in　the　forms　of　amorphous　CaCO3,　calcite,　and　aragonite.　Suitable　early　carbonation　curing　and　subsequent　water　curing　could　increase　CO2　uptake　and　carbonation　depth,　reduce　total　porosity,　and　optimize　the　pore　structure.　CAC　subjected　to　4　hours　of　carbonation　curing　at　20　degrees　C　exhibited　excellent　volume　stability　and　significant　enhancement　of　compressive　strength　up　to　106　MPa　with　90　days　of　subsequent　water　curing.　A　shorter　carbonation　duration　leveraged　the　synergy　between　carbonation　reactions　and　subsequent　hydration　to　enhance　the　macroscopic　performance　of　CAC　significantly.　This　study　offers　new　insights　into　innovative　methods　for　mitigating　the　unstable　transformation　of　hydrates　in　CAC　by　effectively　utilizing　and　sequestering　CO2.