Writing a DVD with a pure UDF filesystem
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K3b (a GUI frontend to mkisofs) can not write to a DVD files larger than 4GB, so you cannot add easily to a DVD a 4.1 GB file (although there is enough space on the DVD). This is due to a limitation of the ISO9660 filesystem, which cannot accept files larger than 2GB (or 4: while Googling it was not very clear whether the limitation is 2 or 4 gigabytes).
So the solution is to burn the DVD using a pure UDF filesystem. Note that K3b cannot currently do that (although it can generate UDF structures, the filesystem is still ISO in the end), so it has to be done via command line. You'll need to emerge udftools and follow the very clear instructions at the following post from the Gentoo forums.