Ninjak and Rai would be my first choice too, the most toyetic of the bunch! Followed by Shadowman and Master Darque. Not as visually interesting, but down the road I'd like Archer and Armstrong. Then Eternal Warrior and Ivar. Not a huge fan of Quantum and Woody, but they'd be visually more interesting... and give us a Goat! Divinity would be neat, and if we get that far Livewire. And the Harbinger Renegades team as a boxed set.
And, since I'm dreaming, a Gold Key (I know, separate license) box set of Turok, Magnus, Solar and Dr. Spektor (I dunno, just throwing a fourth in there).