Mono-　to　few-layer　graphene　materials　are　successfully　synthesized　multiple　times　using　Cu-Ni　alloy　as　a　catalyst　after　a　single-chemical　vapor　deposition　(CVD)　process.　The　multiple　synthesis　is　realized　by　extracting　carbon　source　pre-dissolved　in　the　catalyst　substrate.　Firstly,　graphene　is　grown　by　the　CVD　method　on　Cu-Ni　catalyst　substrates.　Secondly,　the　same　Cu-Nicatalyst　foils　are　annealed,　in　absence　of　any　external　carbon　precursor,　to　grow　graphene　using　the　carbon　atoms　pre-dissolved　in　the　catalyst　during　the　CVD　process.　This　annealing　process　is　repeated　to　synthesize　graphene　successfully　until　carbon　is　exhausted　in　the　Cu-Ni　foils.　After　the　CVD　growth　and　each　annealing　growth　process,　the　as-grown　graphene　is　removed　using　a　bubbling　transfer　method.　A　wide　range　of　characterizations　are　performed　to　examine　the　quality　of　the　obtained　graphene　material　and　to　monitor　the　carbon　concentration　in　the　catalyst　substrates.　Results　show　that　graphene　from　each　annealing　growth　process　possesses　a　similar　quality,　which　confirmed　the　good　reproducibility　of　the　method.　This　technique　brings　great　freedom　to　graphene　growth　and　applications,　and　it　could　be　also　used　for　other　2D　material　synthesis.