Do you want it to last or just something to fill the crack with?
To begin with, it seems like it has settled in all directions, is there any sensible foundation?
Previously, there were holes in the roof and water stood frozen inside the barn, now I have dug it out, insulated, and cast a new slab. Of course, I have repaired the roof and fixed drainage around and installed gutters.
so hopefully it won't settle anymore, so I want to repair the cracks as well and sustainably as possible...
It was probably originally built with mortar B, so it likely works. The alternative is mortar A, which is harder and more similar to the stones. Chiseling out some fresh concrete stone surface in the cracks is probably a good idea - that's what you do when repairing old cast concrete structures with fine concrete to get a grip.
If the wall is moving in the cracks, it will look bad already after one winter.
Plastering concrete stone is a bit beyond my expertise - it might be best to buy a plastering system with instructions. The wall likely needs to be meshed to adhere to the substrate, thinly primed, and then plastered in layers.
regarding the plastering, I've been considering spray plastering, but I have no idea how it works, do you prime the wall? has anyone here done something similar?
No point in doing anything until the settlement damage or rather the cause of it has been addressed. The cracks are shear cracks which are typical in such contexts. Probably requires some form of foundation reinforcement.