Vroom, I totally agree on John Byrne’s Superman and Mike Grell’s Warlord. I would add an absolute of The Longbow Hunters and an omnibus set of Grell’s Green Arrow run.
Ditto on an Infinity, Inc. collection! I’m a big fan of the team. At the very least, I’d like to see a complete collection of “The Generations Saga,” including the All-Star Squadron issues. Then perhaps a collection of the stories featuring Helix (#16-18, 26-29), which feature early Todd McFarlane art.
I second Hawkworld - miniseries and first 25 issues of the main series.
And I’ll add Green Lantern 1990 - issues 1-25. I know there’s rumors about them not being on this service. But the stories are solid and they reintroduced the whole concept of Green Lantern. With that launch pad, Johns wouldn’t have anything to build off of.
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I would love a Showcase Omnibus, The Creeper Omnibus as well of all the Beware The Creepers.
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I would like to see a collection of Archie Goodwin’s editorial run on Detective Comics 437 to 443.
A Superman or Batman silver age omnibus
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Oooh! 
Jonah Hex. That’d be spanking awesome. Can it have nicer paper, not the newsprint kind please. 
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How about Armageddon 2001? There’s more than enough material for an omnibus edition. A lot of those annuals were really good; The Flash, Detective Comics and JLI being some of my standout favorites!