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John le Carré is the natural progression from Graham Greene. Greene wrote several purely thriller novels and several literary ones. Le Carré is sort of a combination of both--just longer and more developed. However, le Carré is almost the complete opposite of Robert Ludlum. Yes, they both have books about international intrigue, but Ludlum is usually a fast-paced, action-packed ride, whereas le Carré's characters spend a great deal of time talking and analyzing. So I guess it depends on what your husband prefers.
If he prefers the literary route, then I'd wholeheartedly recommend le Carré first and foremost. As mentioned above, start with Tinker Tailor Soldier Spy as it contains some possible spoilers for the other two in the loose trilogy, The Honourable Schoolboy and Smiley's People. It's also being (re)made into a movie with Gary Oldman as George Smiley. I think A Perfect Spy is his magnum opus. The Little Drummer Girl, The Russia House, and Our Game are all good, too. His more recent novels are a bit activist in tone, but are still decent. I didn't really care for Absolute Friends, so maybe give that one a miss for now.
You could also try the novels about spies in World War 2 by Alan Furst. He's lighter on plot and a bit sparer, but he's extremely atmospheric.
I also recommend The Turn-around by Vladimir Volkoff, but good luck finding it. You'll have to look in second-hand bookstores.
Vengeance: The True Story of an Israeli Counter-terrorist team by George Jonas, the basis for Spielberg's Munich, is quite interesting, too.
Some people like Len Deighton, but I haven't tried too much of his yet.
If your husband wants the faster-paced stuff, you could try Daniel Silva or maybe Henry Porter. I really don't know what else to recommend here as that's not my area of interest.
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