Stanford and Vanderbilt are in very similar positions. They are both top calibre academic institutions that are very selective and tough to get into. This creates challenges in recruiting for their coaching staffs in that their pool of athletes to draw from is much smaller. This has historically put them behind the pack as far as overall athleticism is concerned.
Harbaugh took that challenge and turned it into an advantage by implementing more complex offenses sets and plays that his players learned to execute very very effectively (having Andrew Luck doesn't hurt either). He also did an excellent job of recruiting and helping players understand where they needed to get academically to gain entrance into Stanford and articulating to them the education and opportunities that would be presented to them through a Stanford education.
Now, could he do the same thing at Vandy? It might be a bit more challenging, due to the depth of the SEC compared to the Pac10, but I think he could do it.
I think he was the most talented offensive coach in college football. Sorry to see him go to the Pros.