Spiderman and His Amazing Friends/ The Incredible Hulk

The earliest appearance of SHIELD on television featured on the final episode of the popular NBC 1980's Spiderman series. Oddly enough neither Nick Fury nor any other regular SHIELD character appears in the episode. This episode does however feature the helicarrier and SHIELD hover cars. Hydra made its first animated appearance in the 1982 animated Hulk series in the episode featuring the She-Hulk.

Spider-Man (1994-1998)
Day of the Chameleon
The Cat (Partners in Danger Part II)
Six Forgotten Warriors, Chapter 1
Six Forgotten Warriors, Chapter 5

With toons like the X-Men, Iron Man, and the Fantastic Four on the air in the 1990s, Nick Fury and SHIELD's guest spots on Spiderman were at the least puzzling, however they serve as the first animated appearances for the stogied hero.
Television actor Philip Abbot voiced Fury for this and the Iron Man animated series, however veteran voice artist Jack Angel took over the role from season 4 onward.

Iron Man (1994-1995)
Not Far From the Tree
The Armour Wars Parts 1 & 2

Tony Stark and Nick Fury go way back in the comics, so its no surprise that when Iron Man nabbed a cartoon for himself Fury popped up a few times. Nick Fury featured in the second season of the series, debuting in the first episode, "The Beast Within" and later in "Not Far From the Tree" and "The Armor Wars" parts one and two. Nick Fury was voiced by actor Philip Abbot. Also worth noting is the first animated appearance of Dum Dum Dugan in "Not Far From the Tree".

The Incredible Hulk (1996 -1998)

Following the success of the X-Men and Spiderman, other Marvel super heroes soon began earning their own cartoon. The Hulk was added to the UPN cartoon lineup and tagging along was SHIELD and Gabe Jones making his animated debut. Voicing Jones was Thom Barry who starred in the Warner Bros film adaption of DC Comics' Steel.

Spiderman Unlimited (1999-2001)

After the Spiderman cartoon wrapped up, the brief spurt of Marvel cartoons also came to an end. Following the success of Batman Beyond, Fox premiered a short-run sequel series to Spiderman where the wallcrawler journeys to an alternate dimension. The premiere episode featured a small part by Nick Fury in the real world. Voicing Nick Fury was Mark Gibbon, who has also voiced Thor (the alien, not the thunder god) on the Stargate: SG1 series.

X-men: Evolution (2000 -2004)

Following the success of the X-Men film, a new animated series premiered on the WB Saturday morning lineup. Following a continuity far removed from that of the Marvel Comics, Logan is known to Nick Fury and SHIELD is guarding the hibernating body of Captain America who is suffering from side effects of the super-solider formula.
Blues musician and actor Jim Byrnes, who played Watcher Joe Dawson on the long running Highlander:The Series voiced Nick Fury.

Ultimate Avengers, Ultimate Avengers 2 (2006)

After years of having to rely on other entities to produce films based on their properties, Marvel at last produced its first animated film, a less adult version of their best selling Ultimates title with Lions Gate Films. As per the Ultimate title, General Nick Fury forms the Avengers as a byproduct of trying to continue the Super Solider program that created Captain America. Actor Andre Ware, voiced General Nick Fury, his second time in the part; the first being in the video game based on the 2005 Fantastic Four film.



Some cartoon images courtesy of the The Un-Official Spider-man Page
thanks to Dan Zadorozny for .gif image. Check out more at his site

Check out this great X-Men Evolution site