When subjecting cast irons to mechanical loading the deformation and damage mechanisms occur on a microstructural level and are dependent on the inherent microstructure. A deeper understanding of the relation between the different microstructural constituents and the macroscopic mechanical behaviour would be beneficial in material development efforts and for the ability to design and cast components with tailored properties. Traditionally, microscopy examinations on sectioned cast iron samples have been used when analysing the microstructure in cast irons. Since all microstructural heterogeneity is in three-dimensions (3D), methods that provide a three-dimensional characterisation are essential for a deeper understanding of, both the microstructural features as well as the deformation and damage of cast irons. Therefore, different cast iron grades have been studied using synchrotron X-ray tomography and 3D x-ray diffraction (3DXRD) at ESRF in Grenoble, France. The samples were stepwise loaded and unloaded in-situ at in the tomography/3DXRD set-up to study the deformation with regard to microstructural constituents and the microstructural evolution in 3D. Based on the 3D tomography image sequences, digital volume correlation (DVC) was used for full strain field analysis and for the analysis of damage and deformation mechanisms. In addition, 3DXRD data were analysed to provide details on the lattice parameters and lattice strain of individual ferrite grains. This work shows the possibilities of such synchrotron experiments for advanced study of the mechanical behaviour of cast iron.