Two choices: East or West. I did East which means navigating the Scoresbysund by sailboat or ship, ideally with reinforced hull. The vistas range from desolate and barren to striking, beyond words beautiful. There are no places to dock but zodiacs will cruise you around bergs and to the shore. I was on a Poseidon ship; topnotch food, facility, staff, guides. Ships depart Iceland unless part of a longer loop, eg Svalbard and more. Easy and recommended to add Iceland if possible; or at least a day on each side to do the Food Walk, Sky Lagoon. Some of my images are on Landscape posted 2023
There are several pros that run tours to West Greenland which has most of the populations, some "cities". Randy Hanna is one (I did TZ safari with him years ago).