The nature of microcracks that developed in concrete is not well understood. One reason for this is the lack of suitable techniques to detect and characterise the microcracks. Conventional methods include imaging polished cross sections with scanning electron microscopy and optical microscopy. However, these techniques only provide a two-dimensional representation of a three-dimensional structure, which significantly reduces the insights from such analysis. Another reason is that the development of microcracks may be associated with various complex forms of concrete deterioration during service life, e.g. due to mechanical loading, drying, thermal effects and chemical reactions. This complicates laboratory scale experiments and inducing “realistic” microcracks in concrete samples becomes very difficult. The aim of this study is to develop new techniques for three-dimensional quantitative characterisation of microcracks and to apply these to understand the properties of microcracks in concrete. A thorough literature review was conducted to identify the causes of microcracking in concrete, mechanisms of microcrack initiation and propagation, transport properties of micro-cracked concrete and methods to characterise microcracks in two dimensions (2D) and three dimensions (3D). Materials and experimental procedures for inducing different types of microcracks, sample preparation for imaging and image analysis of microcracks are discussed. The feasibility of three-dimensional techniques such as focused ion beam nanotomography (FIB-nt), broad ion beam combines with serial sectioning (BIB), X-ray microtomography (μ-CT) and laser scanning confocal microscopy (LSCM) for imaging microcracks were investigated. A new approach that combines LSCM with serial sectioning was proposed to enhance the capability of LSCM for imaging microcracks in 3D. A major focus of this thesis was dedicated to microcracks induced by autogenous shrinkage because this has been previously neglected due to the dominant role of drying shrinkage. Nonetheless, the increasing use of high strength concretes containing low water/binder ratio, complex binder systems and multiple chemical admixtures in recent years has highlighted the problem of autogenous shrinkage in these concretes. This study presents a first attempt on direct characterisation and understanding of the microcracks caused by autogenous shrinkage in 3D. Various concrete samples were produced and sealed cured to induce autogenous shrinkage. The water/binder ratio, cement type and content, and aggregate particle size distribution were varied to vary the magnitude of autogenous shrinkage and degree of microcracking. Linear deformation measurement was performed to correlate autogenous shrinkage with degree of microcracking. Samples were imaged in 2D using laser scanning confocal microscope (LSCM) and in 3D with X-ray microtomography (μ-CT). Subsequently, 2D and 3D image analysis was employed to quantify microcracks > 1 μm in width. A major challenge was to isolate the microcracks that are inherently connected to pores and air voids. Therefore, an algorithm was developed to separate microcracks from pores, and to extract quantitative data such as crack density, orientation degree, distribution of width and length, as well as connectivity and tortuosity. The results show that use of supplementary cementitious materials and low water/binder ratio can increase linear deformation and the amount of the microcracks. The thesis discusses the effect of autogenous shrinkage on the characteristics of the induced microcracking, which is critical to understanding the transport properties and long-term durability of concretes containing supplementary cementitious materials.