Cryo-TEM micrographs of (a) PemFE, 4 mM, and (b) C12FE control molecule, 10 mM, revealing filamentous nanostructures of 9.1 ± 1.4 and 8.5 ± 0.9 nm diameter, respectively. (c) Digital photographs of PemFE and C12FE in a 30 mM 1× DPBS solution after overnight ageing, demonstrating formation of self-supporting hydrogels. (d–f) CEST properties of 10 mM Pem, PemFE, and C12FE at pH 7.4 and 37 °C, with (d) CEST spectra and (e) MTRasym plots of PemFE (solid), Pem (dashed), and C12FE (dotted) showing CEST peaks at 5.2 ppm. (f) Color-coded CEST contrast map of Pem, PemFE, and C12FE with respect to the 5.2 ppm offset from water.