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MOC\u2010based MRI probes increase the relaxation rates of water protons with predominant examples containing high\u2010spin Fe(III). MOC T\n                    <jats:sub>1<\/jats:sub>\n                    MRI probes show enhanced signal based, in part, on slower reorientation times attributed to rigidly linked paramagnetic metal centers. Paramagnetic shift (parashift) probes for MRSI are highly symmetrical MOCs that produce intense paramagnetically shifted proton resonances for improved signal and generally contain high\u2010spin Co(II) or Ni(II). The host\u2013guest properties of MOCs are of interest for the delivery of drugs and for the development of responsive imaging probes to sense small molecules as guests. 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