Here’s a quick analysis of the Letterpress dictionary as of update 1.2.
The Letterpress dictionary is very close to a combination of the CSW12 International Scrabble dictionary plus the ENABLE2K word list. I can’t find an official home page for the latter but here’s a description and link for downloading: http://www.morewords.com/help/.
To these two lists the Letterpress 1.2 dictionary adds the following 137 words: https://gist.github.com/4335238
and deletes the following 141 words: https://gist.github.com/4335247
No word list will please everyone, but the combination of CSW12 and ENABLE2K makes a lot of sense. CSW12 does not include words longer than 15 letters, and although it includes many words that almost nobody has ever heard of it also omits a lot of relatively common words. The ENABLE2K list fills in a lot of the gaps in CSW12, but omits a lot of those peculiar words that Scrabble players have wasted so many hours memorizing. Unlike many of the word lists you can find floating around, both of these lists have been extensively reviewed and edited, so this is an excellent start for an inclusive word list for games like Letterpress.
There are, by the way, two words in the Letterpress dictionary with exactly 25 letters, PHOSPHATIDYLETHANOLAMINES and IMMUNOELECTROPHORETICALLY, so in theory it’s possible to smurf the board on the very first move. Your opponent might suspect you of cheating, however.