We report a novel nanomaterial (AuMN-DTTC) that can be used as a bimodal contrast agent for in vivo magnetic resonance imaging (MRI) and Raman spectroscopy. The probe consists of MRI-active superparamagnetic iron oxide nanoparticles, stably complexed with gold nanostructures. The gold component serves as a substrate for a Raman active dye molecule to generate a surface-enhanced Raman scattering (SERS) effect. The synthesized probe produces T2 weighted contrast and can be used as a SERS active material both in silico (in aqueous solution) and in vivo. A quantitative assessment of T2 relaxation times was obtained using multiecho MRI analysis. The T2 relaxation times of AuMN-DTTC and MN (dextran-coated iron oxide nanoparticles) were 29.23 + 1.45 and 31.58 + 1.7 ms, respectively. The SERS signature of AuMN-DTTC revealed peaks at 508, 629, 782, 844, 1080, 1108, 1135, and 1242 cm(-1). Intramuscular administration of the probe resulted in a decrease of the T2 relaxation time of muscle from 33.4 + 2.5 to 20.3 + 2.2 ms. SERS peaks were observed at 508, 629, 782, 844, 1080, 1108, 1135, and 1242 cm(-1), consistent with the in silico results. Our studies illustrate for the first time the design and in vivo application of a contrast agent, whose component modalities include MRI and SERS. The value of this agent lies in its innately bimodal nature and its application in vivo for molecular imaging applications.