Micro-beads having a carbonaceous structure are produced by a process comsing heating pitch at about 350-500.degree.C to form optically anisotropic spherules, extracting the resulting spherules with an organic solvent to remove substantially all remaining pitch therefrom, and then carbonizing the pitch-free spherules in a non-oxidizing atmosphere. The optically anisotropic micro-beads substantially free of pitch can be shaped to a desired form and then carbonized to produce a shaped carbonaceous structure. If the carbonizing temperature is above about 1500.degree.C, a graphite crystalline structure results.