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BACKGROUND The development of materials with tailored signal intensity in MR imaging is critically important both for the reduction of signal from non-tissue hardware, as well as for the construction of tissue-mimicking phantoms. Silicone-based phantoms are becoming more popular due to their structural stability, stretchability, longer shelf life, and ease of handling, as well as for their application in dynamic imaging of physiology in motion. Moreover, silicone can be also used for the design of stretchable receive radio-frequency (RF) coils. PURPOSE Fabrication of materials with tailored signal intensity for MRI requires knowledge of precise T1 and T2 relaxation times of the materials used. In order to increase the range of possible relaxation times, silicone materials can be doped with gadolinium (Gd). In this work, we aim to systematically evaluate relaxation properties of Gd-doped silicone material at a broad range of Gd concentrations and at 3 clinically relevant magnetic field strengths (1.5 T, 3 T, and 7 T). We apply the findings for rendering silicone substrates of stretchable receive RF coils less visible in MRI. Moreover, we demonstrate early stage proof-of-concept applicability in tissue-mimicking phantom development. MATERIALS AND METHODS Ten samples of pure and Gd-doped Ecoflex™ silicone polymer samples were prepared with various Gd volume ratios ranging from 1:5,000 to 1:10, and studied using 1.5 T and 3 T clinical and 7 T preclinical scanners. T1 and T2 relaxation times of each sample were derived by fitting the data to Bloch signal intensity equations. A receive coil made from Gd-doped Ecoflex™ silicone polymer was fabricated and evaluated in vitro at 3 T. RESULTS With the addition of a Gd-based contrast agent, it is possible to significantly change T2 relaxation times of EcoflexTM silicone polymer (from 213 ms to 20 ms at 1.5 T; from 135 ms to 17 ms at 3 T; and from 111.4 ms to 17.2 ms at 7 T). T1 relaxation time is less affected by the introduction of the contrast agent (changes from 608 ms to 579 ms; from 802.5 ms to 713 ms at 3 T; from 1276 ms to 979 ms at 7 T). First results also indicate that liver, pancreas, and white matter tissues can potentially be closely mimicked using this phantom preparation technique. Gd-doping reduces the appearance of the silicone-based coil substrate during the MR scan by up to 81%. CONCLUSIONS Gd-based contrast agents can be effectively used to create EcoflexTM silicone polymer-based phantoms with tailored T2 relaxation properties. The relative low cost, ease of preparation, stretchability, mechanical stability, and long shelf life of EcoflexTM silicone polymer all make it a good candidate for "MR invisible" coil development and bears promise for tissue mimicking phantom development applicability. This article is protected by copyright. All rights reserved.