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The advent of technologies such as magnetic resonance imaging (MRI)-guided radiation therapy has led to the need for phantom materials that are capable of producing tissue-like contrast on both MRI and computed tomography (CT) imaging modalities. The purpose of this work is to develop a system of easily made and formed materials with adjustable T1 and T2 relaxation times, and x-ray attenuation properties, for mimicking soft tissue and bone with both MRI and CT imaging modalities. The effects on T1/T2 relaxation times and CT numbers were