It's great that this one is brought back up to the top, as I never got around to answering it!
1) Death Duel with the Destroyers: As many have elaborated on, some of the coolest villains, the giant robot, the psychic storm, a cool villain base, the best art of any of the adventures, one of the best covers, etc.
2) FORCE: A fantastic adventure with another cool base, one of the best villains ever, and a great plot.
3) Terror By Night: Another classic villain, cool rules for vampires, a neat setting, and classic monsters.
4) The Island of Doctor Apocalypse: The very best villain for V&V, an undersea base, more giant robots, a cool plot, and an entire island to explore.
5) The Secret in the Swamp: One of the best covers, great art, cool villains, another nifty base, and a unique plot.
Notable mentions to To Tackle the T.O.T.E.M., Dawn of the Devil, Devil's Domain, The Dawn of DNA, Super Crooks & Criminals, and Most Wanted Volume 3.
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