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There's some pretty amazing themes in use, as shown by the great examples posted in this thread :)
Some thoughts came to mind;
1) This is the main XOOPS organization site, the primary. It's look should reflect that. While a lot of the sites posted here have some fantastic visual appeal, if you want a new person to have the first impression that XOOPS is a professionally produced product then the main XOOPS site should convey a professional impression. Get away from 'table borders' and use more white space to separate sections, headers should be very clean and crisp, make more use of different font sizes. Perhaps a top navigation bar for separating major sections so that you are free to use full-width below for sections that deserve more space than a cramped center-column. There's a number of excellent corporate-style themes already contributed here on the site which could be nicely adapted for a custom design. The colours chosen are less important than the style.
2) Since this is the main XOOPS site, it should also be something of a technology demonstrator. It should reflect cutting edge web technology, or at least current state of the art. I know that maximum compatibility is important for the maximum number of users, and maybe that means there should be a theme switch to move between [PLAIN] and [EDGE].
3) I was really impressed by the Zen Garden's examples of what CSS is capable of (thanks Herko!), and I think that this sort of approach could be used to good effect, not just to make the site look better, but as part of the 'technology demonstrator', showing what XOOPS can do with CSS discipline.
4) There's a number of sites that I've admired, but whatever XOOPS uses should be unique to XOOPS. This software isn't like every other package, the site should reflect that uniqueness.
5) The new logo looks great, but using a commercial font forces any graphics designers who want to contribute fully consistant logos or banners either have to purchase the font, or steal it. This seems like an inappropriate position to place people into when all they want to do is contribute their time and talent to a community effort for a free software package. I hope the choice of font is reconsidered.
Just some notions, I hope they're of use.