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 H and F MRI, frequently based on nanomaterials. We will discuss the triggering factors and the strategies employed thus far to activate each probe.