Surface free energy is an important parameter in surface and interface properties of fiber reinforced polymer composite. The BET (Brunauer, Emmett, and Teller) surface area and surface energy of the sample can be obtained by Inverse Gas Chromatography (IGC) based on the adsorption principle. In this paper, surface energy of carbon fiber bundle was tested by means of IGC under different conditions to find reliable test parameters. The main parameters involved include length, mass, and packing density of sample, target fractional surface coverage, flow rate, and maximum elution time. It is demonstrated that IGC has the advantages of simple sample preparation, stable test data, high automation, and high sensitivity for carbon fiber. Among all test conditions, packing density and flow rate have the greatest influences on the experimental results. The optimized test parameters are suitable for various kinds of carbon fiber bundles, including polyacrylonitrilebased and pitch-based carbon fibers with different tensile properties and tow sizes. Moreover, IGC can acutely characterize the surface properties of carbon fibers after carbon nanotube modification and heat treatment, which are hard to carry out using contact angle method.