Abstract: Graphitized carbon foams (GFms) were prepared using mesophase pitch (MP) as a raw material by foaming (450 °C), pre-oxidation (320 °C), carbonization (1000 °C) and graphitization (2800 °C). The differences in structure and properties of GFms prepared from different MP precursors pretreated by ball milling or liquid phase extraction were investigated and compared, and semi-quantitative calculations were conducted on the Raman and FTIR spectra of samples at each preparation stage. Semi-quantitative spectroscopic analysis provided detailed information on the structure and chemical composition changes of the MP and GFm derived from it. Combined with microscopic observations, the change from precursor to GFm was analyzed. The results showed that ball milling concentrated the distribution of aromatic molecules in the pitch, which contributed to uniform foaming to give a GFm with a uniform pore distribution and good properties. Liquid phase extraction helped remove light components while retaining large aromatics to form graphitic planes with the largest average size during post-treatment to produce a GFm with the highest degree of graphitization and the fewest open pores, giving the best compression resistance (2.47 MPa), the highest thermal conductivity (64.47 W/(m·K)) and the lowest electrical resistance (13.02 μΩ·m). Characterization combining semi-quantitative spectroscopic analysis with microscopic observations allowed us to control the preparation of the MP-derived GFms.