The goal of this research was to demonstrate the potential of spectral CT for the discrimination of vulnerable atherosclerotic plaques. It was proposed that spectral CT has the potential to identify the presence of specific markers for vulnerable plaques: iron deposits and lipid core. A spectral micro-CT system incorporating the latest Medipix spectroscopic photon- counting detectors was commissioned for this purpose. Using spectroscopic methods developed with this system, it was possible to distinguish the presence of iron deposits and lipid core within ex vivo atherosclerotic plaques. Atherosclerosis or hardening of arteries is a systemic disease of the vessel wall that occurs in the aorta, carotid, coronary and peripheral arteries. It is characterised by the deposition of calcified plaques on the innermost layer of the artery wall. Vulnerable plaques are unstable, prone to rupture and put the person at risk of cardiovascular events and strokes. Factors that may lead to plaque instability are lipid content and iron deposits. This preclinical study is a precursor to the development of a clinical technique that will enable vulnerable atherosclerotic plaques to be identified in vivo prior to treatment or removal. Following a preliminary study on atherosclerotic plaques with a prototype system, the MARS-CT3 spectral micro-CT system incorporating Medipix3 was developed and commissioned for further plaque studies. The spectral CT data sets acquired by this system were assessed visually for morphology and analysed for material composition using a linear algebra method. The results were correlated with photography and histology (the histology is the current gold standard). The presence of iron and lipid can be differentiated from the background soft-tissue using a linear algebra method. However the quantification of iron in the presence of calcium is not currently possible without additional data or constraints. Nevertheless the presence of iron deposits within the plaques can be distinguished in the high resolution MARS-CT images and has been correlated with photographic and histological evidence. Thus, using the high spatial resolution spectral data from MARS-CT, the discrimination of lipid core and iron deposits within ex vivo advanced human atherosclerotic plaques is feasible. This may provide the basis for the development of a clinical technique that will identify vulnerable plaques in vivo by high resolution spectral CT.