Magnetic resonance imaging (MRI) is a non-invasive imaging technique with widespread use in diagnosis. Frequently, contrast in MRI is enhanced with the aid of a contrast agent, among which smart, responsive, OFF/ON or activatable probes are of particular interest. These kinds of probes elicit a response to selective stimuli, evidencing the presence of enzymes or acidic pH, for instance. In this review, we will focus on smart probes that are detectable by both 1H and 19F MRI, frequently based on nanomaterials. We will discuss the triggering factors and the strategies employed thus far to activate each probe.