Take a look at some of these:
The New Adventures of Batman (1977) - this was done at the same time as the Superfriends, and it showed more of the Batman from the comic books of the 1970s. It had Adam West and Burt Ward doing the voices, but it didn't have the campiness of the 1960s TV show. And I don't care what anyone says, I did NOT think Batmite was the devil!
The (New) Adventures of Superman (1966) - along with the follow up The Superman/Aquaman Hour, these shows were awesome. With narration by Ted Knight, plus the first appearance of Superboy in a cartoon
Battle of the Planets (1978) - my first exposure to anime. (fuck Speed Racer, THIS is what it's all about). A redub and remix of the Japanese show Gatchaman, I could even deal with that R2D2 ripoff, 7-Zark-7. This has probably the best orchestral theme song for a cartoon that I have ever heard.
Courageous Cat and Minute Mouse (1960) - a furry-animal version of Batman and Robin, from the guy who created the original. Another very catchy theme, almost a ripoff of Peter Gunn.
Danger Mouse (1981) - I went to school with someone who named their hampster "Penfold". When are they going to release this on DVD?
The Fantastic Four (1967) - I never really read Marvel Comics when I was a kid, so my exposure to Stan Lee's universe came from this show. I just loved the Thing. Hell, I even liked this show, although I think I was the only one.
In the same vein, The Incredible Hulk (1966) - everyone piles abuse on this one and the other Marvel heroes this animation studio did (Captain America, Sub-Mariner, Ironman), but I kind of like it. I have to agree, though, the version from 1982 is a lot better.
Fastastic Voyage (1968) - I liked this better than the movie, but I was a little kid and didn't have the adult appreciation of Raquel Welch. I haven't seen this in years, but I remember Guru, the token Indian, doing all sorts of levitation and mind-reading with just the wave of a hand.
George of the Jungle (1967) - I don't actually remember this cartoon, but it is another one with a killer theme (Two, acutally, becuase it also had Super Chicken). The live action movie 30 years later is one of my alltime favorites, if for no other reason than for kick-starting Brendan Fraser's career.
The Herculoids (1967) - for some strange reason, I always tried to do the voice of Gloop and Gleep. I just thought they sounded cool.
Kid Super Power Hour with Shazam! (1981) - man, I'm really reaching with this one. It had a live action part (Hero High) which was absolutely terrible, but the Shazam cartoon was actually pretty good. If they could have kept that and ditched the rest, I would have been a happy adolescent. (BTW, the theme for this sounds like exactly what it is: an actor who thinks he can sing but really can't).
The Mighty Hercules (1963) - I remember watching this on UHF 69 in New Jersey (don't remember the call letters - if someone can help me out), right before Uncle Floyd. Cheap as hell animation, but I remember it after all these years, so it must have had some redeeming value.
The Mighty Mightor (1967) - it's a good thing this was made by the same people who made Captain Caveman. Otherwise, the writers of this show would have a hell of a lawsuit. A caveman superhero, complete with power club. I think this was aroudn the same time as Birdman, Herculoids, and a shitload of other Hanna-Barbera superhero cartoons.
Samson and Goliath (1967) - I remember watching this on the USA Network Cartoon Express. You gotta know this was a precursor to He-Man. Obscure fact: Tim Matheson, Otter of Animal House fame, was the voice of Samson (as well as Johnny Quest, and Jace from Space Ghost).
Shazzan! (1967) - (in a bad Beavis and Butthead voice) "The camel is named Kaboobie." "Heh, heh. The camel's hump looks like a big kaBOOBIE." What do you want from me, I was a kid!
Spider-Man, in both the 1967 and 1981 versions. The '67 one was just released on DVD (BTW, does it have the cover version of the theme by the Ramones?), but the other one is lost in obscurity. I just loved the opening monologue by Stan Lee.
Star Blazers (1979) - I have a confession. I never watched this when I was a kid, and I didn't really get into the series when I was older. However, it has got the second best anime theme I've ever heard (see above), very much a battle march. I remember my Ren-faire friends and I drinking massive amounts of beer while listening to it.
Star Trek: the Animated Series (1973) - The bridge between the original TV series and the first movie. Almost the entire original cast was back (no Chekov or Walter Koenig), and they even managed to get some more aliens on board (the lioness communications officer, the three-armed, three-legged navigator). Plus, I love Filmation's dramatic music.
Tennessee Tuxedo (1963) - Before he was Inspector Gadget, even before he was Maxwell Smart, Don Adams was a sneaky penguin. I probably learned more from Doctor Whoopie than I from any other TV cartoon (except maybe for the end of GI Joe). Of course, I can't mention Tennessee Tuxedo without mentioning...
Underdog (1964) - All you have to do is look at my icon, and know that I love this little guy. He also had the best criminal names (Simon Bar Sinister, Riff Raff).
Of course, this isn't a complete list. I've left off the obvious ones from the early and mid 1980s (Transformers, GI Joe, Voltron, etc) because they never really faded into obscurity like the others, and to be honest, by that point all they were used for was to sell toys.