The optimum carbonization conditions for converting a low-sulphur petroleum vacuum residue in a tube bomb in terms of pressure and temperature into better needle coke of low CTE, with less production of poor bottom coke, were studied by observation of the resultant cokes and sequential analyses of carbonization intermediates by means of solvent fractionation and gas evolution. Carbonization at 460°C under 15 kg cm−2 G produced the best needle coke. The quality of the resultant needle coke was strongly influenced by viscosity changes of the system, the solidification range and gas evolution in the carbonization progress. The first two characteristics reflect the rates of condensation (such as QI formation) and devolatilization of soluble fractions, strongly influencing the growth of anisotropic units. The last characteristic reflects the pyrolytic cracking reaction to define the timing of gas evolution during carbonization, influencing the axial orientation of anisotropic texture as well as the porosity in the resultant coke. Both profiles varied very much, depending on the carbonization temperature. Finally, the formation of a bottom coke of fine mosaic texture is discussed from the viewpoint of the co-carbonization concept.