In the later primaries, Santorum got many more votes than Gingrich, so if Romney's main concern was to reassure conservatives, Santorum would be a better bet. Not that I think there is much chance of Santorum being chosen...there are other candidates who can reassure conservatives plus win independents and help win their own state (Santorum doesn't put his own state firmly in the Republican column).
IMHO, either Sarah Palin (if she’s willing to do so again) or Jim DeMint would be the best choices for VP, if Mitt, really, wants to excite the conservative voters base, to the best of abilities.