The Flintstones Season 4. I'll probably get the "Huckleberry Hound" set, pass on "Flintstones," and consider "Yogi Bear."
With Hanna-Barbera cartoons, the earlier the better; the earliest cartoons have some fine animation within the limited budget, and stories that are reminiscent of classic Warner Brothers cartoons, mostly because they hired the classic WB cartoon writers, Warren Foster and Mike Maltese. As their shows get more like sitcoms, I lose interest. (I know the early Flintstones have some good things and are quite well-animated, but compared to The Honeymooners it's really just a collection of old-school sitcom plots with an occasional clever satirical joke thrown in.) And oddly enough, I like Hanna-Barbera's early TV cartoons a lot more than I like their MGM work -- funnier and less mean-spirited, and with more distinctive characters than Tom or Jerry ever were.
I also seem to remember that some of the early Yogi Bear cartoons, when he was on the Huckleberry Hound Show, had him as an obnoxious wise guy like Bugs Bunny, though I'll have to refresh my memory when I see the set as to how often he acted like that; I saw one which was basically a Bugs story with Yogi in it, but that might have been a one-off, or Foster or Maltese burning off a story they didn't get to use at Warners.
And for an indication of how popular "Huckleberry Hound" was, here's a quote from a 1959 recording by Canadian comedians Wayne and Shuster (and for any Canadian viewers with unfond memories of them, let me assure you that they were very funny back in 1959) of their routine "I Was a TV Addict":
SHUSTER: Come on, I've made an appointment for you with the psychiatrist. It's at five o'clock.
WAYNE: Five o'clock?!
SHUSTER: What's the matter?
WAYNE: I'll miss Huckleberry Hound!
SHUSTER: Aw, come on!
WAYNE: And Yogi Bear!