The nanostructure, fractal dimension and size of in-cylinder soot during diesel combustion process have been investigated for a heavy-duty direct injection diesel engine, using a total cylinder sampling system followed by high-resolution transmission electron microscopy and Raman scattering spectrometry. Different structural organizations of in-cylinder soot are found depending upon the combustion phase. It is revealed that both the fringe tortuosity and separation distance decrease as combustion proceeds, while the mean fringe length increases distinctly from 1.00 to 2.13 nm, indicating the soot evolution toward a more graphitic structure during the combustion process. The fractal dimensions of aggregates are in a range of 1.20-1.74 at various crank angles under the applied engine operating conditions. As temperature and pressure increase, the fractal dimension decreases significantly to a minimum at the early diffusion combustion stage. The soot particles become more compact again as the fractal dimension increases during the subsequent combustion period. Primary particle sizes start small, go through a maximum in the early diffusion combustion phase and decline again as combustion proceeds. (C) 2010 The Combustion Institute. Published by Elsevier Inc. All rights reserved.