Here we report on a dual-modal 19F and 1H MRI paramagnetic probe with a self-immolative linker, GdDOMFGal. The enzymatic conversion of this probe by beta-galactosidase resulted in a simultaneous turning on of the fluorine signal and changed ability of the Gd3+ complex to modulate the 1H MR signal intensity of the surrounding water molecules. A versatile imaging platform for monitoring a variety of enzymes by 19F and 1H MRI using this molecular design is proposed. Copyright (C) 2012 John Wiley & Sons, Ltd.