The influence of aggregate size and water-to-cement (w/c) ratio of the matrix on the structure of interfacial transition zone (ITZ) and the interaction between the ITZ and the matrix on the failure process of concrete under uniaxial compression were studied. The ITZ microcracking and the failure process of concrete were investigated experimentally by means of compressive and indirect tensile testing, stress-volumetric strain measurements and microscopic analyses on the model concrete containing single spherical steel aggregate with three different w/c ratios. At low w/c ratios, the rigid and smooth surface texture aggregates made by the ITZ have a significant structural difference compared to the mortar. This was more pronounced for larger aggregates. Higher structural differences between the mortar matrix and ITZ in low w/c ratio composites resulted in accelerated ITZ microcracking at high stress level. The effect of condensed microcracking in a narrower ITZ was reflected in the lower critical stress levels for the low w/c ratio composites with larger aggregates. (C) 2004 Elsevier Ltd. All rights reserved.