We introduce gas vesicles (GVs), a class of gas-filled protein-only nanostructures discovered in photosynthetic microbes. While the air-to-water magnetic susceptibility difference enables their T2/T2* contrast, their unique acoustic property allows the use of sub-millisecond ultrasound pulses to erase the contrast in situ, which enables background-free MRI. GVs can be used as reporter genes to image biological processes in living bacteria. Genetic variants of GVs, differing in their magnetic or mechanical properties, allow multiplexed imaging using parametric MRI or differential acoustic sensitivity. Finally, clustering-induced changes in MRI contrast enable the potential design of dynamic molecular sensors. These protein contrast agents, possessing dual responsiveness to MRI and ultrasound, give rise to a new modality for molecular imaging with unique capabilities and advantages.