The search for higher spatial resolution and better sensitivity stimulates the development of high-field (3 T) and ultrahigh field (>3 T) MRI scanners. Gadolinium-based MRI contrast agents, commercial ones used in clinics, as well as recently developed more efficient ones, become less and less effective as the magnetic field is increased above 3 T and, therefore, special contrast agents for ultrahigh-field MRI have to be developed. As the relaxivity, defined as relaxation enhancement per Gd-ion, is rather limited, marked boosts in performance can only be achieved by creating systems transporting many paramagnetic centers to the desired site. To obtain maximum efficiency gadolinium chelates with more than one water molecule in the first coordination sphere must be used. The rotational correlation time should be in the range of 0.5–1 ns and the residence time of first sphere water molecules should be short (<10 ns).