Sugar‐based biopolymers have been recognized as attractive materials to develop macromolecule‐ and nanoparticle‐based cancer imaging and therapy. However, traditional biopolymer‐based imaging approaches rely on the use of synthetic or isotopic labeling, and because of it, clinical translation often is hindered. Recently, a novel magnetic resonance imaging (MRI) technology, chemical exchange saturation transfer (CEST), has emerged, which allows the exploitation of sugar‐based biopolymers as MRI agents by their hydroxyl protons‐rich nature. In the study, we reviewed recent studies on the topic of CEST MRI detection of sugar‐based biopolymers. The CEST MRI property of each biopolymer was briefly introduced, followed by the pre‐clinical and clinical applications. The findings of these preliminary studies imply the enormous potential of CEST detectable sugar‐based biopolymers in developing highly sensitive and translatable molecular imaging agents and constructing image‐guided biopolymer‐based drug delivery systems. This article is categorized under: Diagnostic Tools > in vivo Nanodiagnostics and Imaging Therapeutic Approaches and Drug Discovery > Emerging Technologies With the magnetic resonance imaging (MRI) technology of chemical exchange saturation transfer (CEST), sugar‐based biopolymers can be directly used as novel imaging agents for a broad spectrum of biomedical applications.