Cryptophane cages are very promising for (129)Xe-MRI. These molecular cages are extremely hydrophobic, which currently limits their use for diagnostic applications. To overcome this, the synthesis of water-soluble dendronized cryptophanes with surface groups for further functionalization is reported here. These molecules retained all the "core properties of cryptophane" that are crucial for biosensor applications as analyzed by Hyper-CEST imaging and spectroscopy. This approach is promising for developing new generations of xenon-cryptophane-based biosensors.