My favorite Connery movie ever is Robin and Marian (1976), which imagines what happens when Robin Hood comes returns from two decades on the Crusades to a Nottingham in which he's been turned into a myth.
Richard Harris plays Richard the Lionheart as an addled, vicious despot and the movie's Crusades are a genocidal, pointless war of empire, and that's just the first fifteen minutes.
When Robin gets back to Nottingham, he reconciles with Marian—a transcendent, angry, and age-appropriate (!) Audrey Hepburn in one of her last roles—and tries to construct a life of meaning and honor out of the pieces of his legend.
The movie is almost forgotten now, but it's sweet and sad and powerful in a very seventies way, and maybe Connery's most thoughtful commentary on the Bond movies, too. It's a joy.
Oh, and spoiler: 
Herewith my favorite of all the (many, many, many) times I've mentioned Robin and Marian on Twitter:
https://twitter.com/studentactivism/status/895428484620800000
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