A method for forming a vapor-grown graphite fibers (VGGF) composition and a VGGF composition formed by the method are provided. In this method, a transition metal compound catalyst and three organic co-catalysts are mixed with a hydrocarbon compound, and then are delivered into a tubular reactor and pyrolized and graphitized to produce the VGGF composition. The VGGF composition includes a carbon ingredient containing a carbon content of at least 99.9 wt %. The carbon ingredient has a graphitization degree of at least 75%, and the carbon ingredient includes non-fibrous carbon and fibrous VGGF, wherein an area ratio of the non-fibrous carbon to the fibrous VGGF is about equal to or smaller than 5%. The fibrous VGGF include graphite fibers having a 3-D linkage structure, wherein the content of the graphite fibers having the 3-D linkage structure in the fibrous VGGF is about between 5 area % and 50 area %.