What is the best way to fix a crown molding joint that has separated?




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Caulking.
Most use a caulk that is paintable to repair joint separation. Make sure to check structure first that now attachment nails/staples are loose and need to be repaired. Click on the links below for "how to" repair joint separation.
https://www.youtube.com/watch?v=k4EZFf4rmsk
http://www.contractortalk.com/f13/crown-molding-pulling-apart-reveal-seam-110232/
https://www.youtube.com/watch?v=GdaZtOZyKz4
use some silicone calking to fill the gap, then touch up paint to match