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Chemical exchange saturation transfer (CEST) magnetic resonance imaging (MRI) is an innovative molecular imaging technique in which contrast agents are labeled by saturating their exchangeable proton spins by radio‐frequency irradiation. Salicylic acid and its analogues are a promising class of highly sensitive, diamagnetic CEST agents. Herein, polymeric agents grafted with salicylic acid moieties and a known high‐affinity ligand targeting prostate‐specific membrane antigen in approximately 10:1 molar ratio were synthesized to provide sufficient MRI sensitivity and receptor specificity. The proton‐exchange properties of the contrast agent in solution and in an experimental murine model are reported to demonstrate the feasibility of receptor‐targeted CEST MRI of prostate cancer. Furthermore, the CEST imaging data were validated with an ¹¹¹In‐labeled analogue of the agent by in vivo single photon …