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When I first saw Syndrome, I immediately thought he should be voiced by Donal Logue from ER. :D (http://imdb.com/name/nm0006610/maindetails)

Any new fans of Sarah Vowell might enjoy checking out Gigantic (A Tale of Two Johns), the documentary about They Might Be Giants. She has quite a bit of on-screen time, as far as I recall, and her comments are very interesting as well.