One suggestion is to put up a tamp. The shadows around the tamp remove some irregularities in the walls. But if it becomes discreet... hmm, maybe not.
 
Make a cone like the baker filled with husfix in the right consistency, then pipe it into the gap between the wall and ceiling. Husfix can be painted over with silicate paint if that's the type of paint you have in the basement today.
 
Leave it with some gaps. We applied fake brick on our chimney breast and since it became somewhat smaller and also uneven, I was a bit doubtful if it would look good with crown moldings. However, I just placed it, and the gap is quite large, but no one notices it today (not even me).

This image shows how it turned out even if it doesn't focus on the actual crown molding.
http://hus.jarkeborn.se/index.php?option=content&task=view&id=13&Itemid=30
NOTE: The site is under construction!!
 
Otherwise, you can always install a cornice and fill the gap against the wall with construction silicone (paintable!) and paint the whole thing...
 
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