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.