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Things such as gparted are supposed to handle this, but I've never got a GUI to handle it properly.
I'd suggest you use ntfsresize from the ntfsprogs package, and reduce the NTFS. There is a very good page on the project site with plenty of info.
Rather than trying to resize the Ubuntu as well, think about creating a new partition, and mount your biggest directory there - say /media/mp3s or whatever.
Simple generally works best.
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