I've always gone with Alyson Hanigan for Theriault. I believe she was David Mack's pick, and I've never really been able to picture anyone else.
I didn't really follow her earlier work (e.g. Buffy, American Pie), so my mental impression of her (approaching 40) is too old for the character (though she certainly looked the part c. 2005, despite being over 30).
Vanessa Theriault - Molly Quinn (Alexis Castle on Castle; semi-recent interview - spoilers for season 6)
I like Molly Quinn a lot, but don't you think she's a bit young? Granted, Theriault starts as an ensign in the stories set in 2266, but she's a lieutenant j.g. by 2268 and a lieutenant commander by 2269. Quinn only just turned 21--she's literally not even old enough to have graduated from college yet on a traditional college schedule. And she looks it.
I was thinking more of early-Vanguard Theriault. While Quinn is probably still a little young, I find mentally aging her a year or two easier than imagining a younger Hanigan. (Theriault seems like the type who might have skipped a year along the way somewhere, anyway.)
Her age by the time of Seekers would be about 26* without mentally adjusting, anyway, which isn't terrible for a rapidly-promoted LCDR in the context of some of Star Trek's other promotions (27-year-old Captain Kirk, 18-year-old Chief Engineer Chekov, 28-year-old Captain Picard).
*I went with "Turnabout Intruder" as being near the end of the five-year mission (no TAS), rather than the 6-8 months earlier date used in the novels, but the difference probably isn't ultimately all that material.
Edit: Huh, just discovered I wasn't the first person to suggest her.
I like a lot of David Mack's choices for the Vanguard characters. (I see a few differently, though.)
Diego Reyes - Edward James Olmos
Rana Dasai - Parminder Nagra
Dr. Fisher - Morgan Freeman
Cervantes Quinn - Stanley Adams
Ming Xiong - Jet Li
Lurqual - Katherine Heigel
Ganz - Ving Rhames
Oriano D'Amato - Monica Belucci
Atish Khatami - Catherine Bell
Aledard Nassir - Ben Kingsley
Vanessa Theriault - Molly Quinn (in a few years)
Not sure I agree with Quinn as Colt (mooted farther down the page), though.
Inspired by Tara casting her as Caitlin Barry in her nu-Pike fanfic, what about Gina Holden as Bridy Mac?
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