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X-Men: The Animated Series and Spider-Man: The Animated Series were both quite good.
Batman: TAS is a classic; probably one of the finest television series to ever grace the small screen.
My personal favorite is Justice League Seasons 1 and 2 (Unlimited got too convoluted and wasn't enough about the main 7 anymore). There are some great episodes like "A Better World" (a control obsessed Justice League from an alternate universe enters our Earth, kidnaps the JL and takes over), "Starcrossed" (Hawk People invade Earth and Hawk Girl is revealed as a traitor), "War World" (Superman is captured by Mongul and forced to battle on War World), and "The Savage Time" (the JL has to go back in time to WWII and help defeat Vandal Savage - a computer genius who traveled back before them, usurped Hitler, and used revolutionary technology to win WWII).
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