Graphene has attracted much attention since its first discovery in 2004. Various approaches have been proposed to control its physical and electronic properties. Here, it is reported that graphene-based intercalation is an efficient method to modify the electronic properties of few-layer graphene (FLG). FeCl3 intercalated FLGs are successfully prepared by the two-zone vapor transport method. This is the first report on full intercalation for graphene samples. The features of the Raman G peak of such FLG intercalation compounds (FLGIC) are in good agreement with their full intercalation structures. The FLGICs present single Lorentzian 2D peaks, similar to that of single-layer graphene, indicating the loss of electronic coupling between adjacent graphene layers. First principle calculations further reveal that the band structure of FLGIC is similar to single-layer graphene but with a strong doping effect due to the charge transfer from graphene to FeCl3. The successful fabrication of FLGIC opens a new way to modify properties of FLG for fundamental studies and future applications.