1)
What is the significance of "Bein Gevul Yehudah u'Vein Gevul Binyamin"?
1.
Rashi: The entire width between Yehudah in the north and Binyamin in the south, will be to the Nasi.
2.
Radak: Above it mentioned the seven Shevatim to the north of the Nasi's portion. Here it says that the Nasi's portion is between Yehudah and Binyamin, and below it lists the other four Shevatim in the south.
2)
Why does the verse teach about Achuzas ha'Leviyim and Achuzas ha'Ir?
1.
Malbim: Also they are in the middle of the Nasi's portion. It is as if the Nasi separated them from his portion.