Here's a smattering of recommendations...
The Wild Wild West: If the only thing you know by this name is the Will Smith feature film monstrosity from a few years back, please see the original '60s TV series to wash away the foul taste. Very quirky and hip... it holds up very well, thanks to fine scripting and acting. Only the first season is available so far, but the second is due soon.
Walking With... whatever they got! "Dinosaurs", "Beasts", "Cavemen", "Monsters"... the last word in televised paleontological reconstruction! These BBC produced series feature an intelligent, literate approach that bolsters the stunning CG visuals. My cherished prehistoria has never seemed so real! Watch for "Allosaurus, the Ballad of Big Al", and "Chased by Monsters", more lively goodies from the same producers.
The Outer Limits: The original '60s season-and-a-half, not the later abortion. The best of bizarre storytelling in bold, beautiful black-and-white! Taut, lyrically written, well acted (by performers who would later become TV icons) and directed with high visual flourish. The Joseph Stephano episodes (he produced the first season and also scripted) have a faux-Shakespearean lilt that's like music to listen to! Not easy to find anymore, though I've seen used copies reasonably priced.
Rocky and Bullwinkle: The immortal Jay Ward classic! Three seasons are available, not all by a long shot, but it's been a long time since the last release. I fear the schedule may be at an end... what a crime! This series is a marvel of sassy brilliance, filled with crazed scenarios, iconic characters and topical quips that seem no less fresh today then when they were new. The animation style makes the most of meager resources, turning production paucity into a virtue! Precious little Jay Ward stuff has made its way to DVD (if you don't count pirate copies, where it's raving popular)... enjoy what there is while it lasts.
Also looking forward to the upcoming release of Get Smart, a hilarious spy spoof from (yet again) the 1960s. My treasured childhood will live again if I have to force it!