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Where my ceiling drywall meets a brick wall there is a gap.
This is smaller at the brick itself (maybe 3/16") and then larger where the mortar is struck.

This seems too large to fill with caulking... what about using drywall compound?

EDIT: I should clarify that I have access to both sides of this gap, from the attic. In case that makes a difference.

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    I think this is why they invented Quarter round. You also might want to consider some fancier Crown Molding. – Tester101 Aug 30 '12 at 15:17
  • @Tester101 I considered that, but I thought it might look strange having a quarter-round at the top of the brick, and no crown elsewhere in the house (this is a ranch-style home with relatively low ceilings). – Matthew Aug 30 '12 at 15:37
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Drywall compound by itself might not be the best solution since its not really a great gap filler; it requires a backing to adhere to which is why you use either paper or fiberglass tape when putting up drywall.

As tester101 suggested, you could use crown molding or quarter round to cover it up.

I would imagine that filling it with mortar might give the most natural looking results since mortar is already used and it would blend well with the overall appearance.

Alternatively, I think you could fill this with a paintable caulking or spray foam - it really depends on the results you are going for. With caulking you are still likely to see the gap - it will just be filled with a different material now.

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If you want to fill a large gap with caulk, the first thing you do is fill the gap with a caulk "backer rod" that's made of foam. They come in various diameters are are typically found near the weather stripping in a home improvement store. You shove the backer in with a putty knife (not too deep, just enough to be below the surface), and then cover with caulk.

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