David Louis Edelman asks "what are some quality SF books you can hand off to literate non-SF readers as an introduction to the genre?"
It's a fantasy any specfic person has, and I've had it plenty. If you're going to try to get a literary reader, I would agree absolutely with a few of the commenters that short stories would be the place to start. My recommendations: Delaney's "Aye and Gomorrah," Harlan Ellison's "Jeffty is Five," Bob Shaw's "Light of Other Days," and China Mieville's "Reports of Certain Events in London."
But say that works, and they like one or more of the stories above. Is that going to have them poring through Zelazny's works? Probably not. I think the flaw in thinking here is the assumption that "literary" people just assume that any counterfactual effects in a story automatically make it non-literary, and if we could just get them over thinking that then they'll be showing up at ReaderCon next.
But this is obviously not the problem, or else we wouldn't see Jonathan Lethem, David Foster Wallace, J.G. Ballard, Margaret Atwood, Italo Calvino, Richard Powers etc., etc., stacked on the "Literary" shelves instead of "Science Fiction." It is entirely possible, even likely, that a literary reader would say "I accept that a work of literature can have science-fictional elements, or even be science fiction. But that isn't going to make me a science fiction reader." If a literary reader finds a scifi book that he likes, he's more likely to file that person and/or story under the exceptions to the rule column.
I can actually understand this. I like Elmore Leonard's books a lot. He's a hell of a storyteller, and I've read 4-5 of his books. But these books have increased my interest in the rest of crime fiction (or whatever his genre is) by exactly 0%. I bet there are all kinds of people who love Walter Mosely and have never touched another mystery novel in their lives.
For a person to become a science fiction reader, they are just going to have to have an interest in the kind of topics that scifi addresses. These would include directions in future technology and how it would affect humans, interstellar travel, contact with non-human sentiences and alternate social constructs under counterfactual situations. As much as I love Alastair Reynolds, and as brilliant as he is, his work just isn't going to be all that interesting (or even make much sense) unless you've thought awhile about relativity. Not that you have to be an expert; but unless you understand what relativistic velocities do there's just too much catching up there.
In truth there are already a lot of literary people who have secret genre habits, and I'd suspect the two biggest would be mystery and scifi. Winning "regular readers" over to scifi is the bigger challenge, I agree. We've got a long way to go.