The first
Cyborg 009 show from 1968 is an absolutely awesome watch. The artwork and character design is fantastic, there's loads of hilarious comedy with 006 and 007 (who's very different from the other interpretations of the character, and is voiced excellently by the chick who played the original Rita Repulsa), and some of the plots are INSANE! (But great!) It's cartoony, dramatic and theatrical, action-packed, and just an awful lot of fun. I love how they drew anime characters back then.
Aaah-aaah, Cyb-oooorg, zero-zero-niiiiine...
I've also seen the two movies based on this series, the first of which predates it (and is one of the very first feature-length anime movies ever). They're great, too! The only problem is that the guy subtitling this dumb show takes FOREVER to put out now eps. WHAT A JERK!!!!
And if you want to go earlier than that,
Sabu to Ichi Torimono Hikae is just a fucking beautiful series from start to finish. It's a quiet, contemplative "cop show" set during the Jidai Geki starring a righteous young samurai and his blind masseuse mentor. Both characters are just realized fantastically – they're entertaining, charming, and the sort of honourable that you can look up to.
There's loads of action against evil criminal ninjas and cackling villains and the like, but there are also many gentle, ruminative moments where you can just chill the F out with the characters. Sabu and Ichi have a wonderful "knowing father/upstart son" relationship that makes them both really endearing, as does the very theatrical relationship between Sabu and his bride-to-be. I've watched this show before I gone to bed in the dead of night many times, and it just puts you in a really relaxed, mellow, happy mood.
It's also an anime series that came out so early that they didn't even know how to do a lot of animation techniques in the first several episodes, so you'll get things like water being actual, live-action footage of a pond with character drawings project onto it. Animation is limited, but it's so cool to think about it in relation to where anime has come in the following six decades. I love this show to bits.
And finally, if you're looking for a great '60s anime movie,
The Flying Phantom Ship is right up your alley. It's a fun adventure film about a mysterious ghost ship that appears over Japan, and the only two meddling kids (and their dog!) that cane save the day. It's packed to the brim with ghosts, monsters, skeletons, giant robots, explosions, angry politicians, aerial battleships, and heart.
Anime fans will also be interested to know that this movie was a certain Hayao Miyazaki's very first animation job – he designed the giant robot in it! The characters are all cute and kooky, there's plenty of action and comedy, and the colouring is immaculate – total '60s chic. Very much recommended if you're after an hour or so of classic anime fun.
I love, love, love '60s anime. Oh my god, so much of it is exactly what I want out of animation. I have examples from the '70s, too, but I'm going to hold my little tongue for now – this thread is great!