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The Mandarin first appeared in the comic book Tales of Suspense #50 (from February 1964), and was created by Stan Lee and Don Heck. The man who became known as the Mandarin was apparently a descendant of Genghis Khan who found the ruins of a star-ship that crashed on our planet centuries earlier. He discovered ten rings (which were supposedly the power source for the ship), and by wearing these rings he gained new powers. He managed to understand and master the technology from the ship, and went on to become a conqueror - he subjugated many of the villages surrounding the so-called valley of Spirits from China and with his knowledge of science rapidly became a power that not even the Chinese Army could successfully challenge. His plans did not end here though as he wished for world domination, but all of his schemes were thwarted by Iron Man. The armored avenger was the main obstacle in the Mandarin's plans for world domination.
His first animated appearances were on the Marvel Super Heroes Show, which aired in syndication in 1966 and featured five of Marvel's superheroes starring in their own series each one consisting of 13 episodes (separated into three 7-minutes long segments). This show had very limited animation, and was composed almost entirely of actual comic book panels with a voice-over; basically an early version of today's motion-comics. The Mandarin here was voiced by Bernard Cowan (using a strong accent) and primarily appeared on the Invincible Iron Man segments: he appears in a total of four Iron Man episodes - and is one of the few major villains that appeared more than once (the others being the Crimson Dynamo and the Titanium Man, who each appeared in two episodes) - and also briefly appears in one episode of the Namor the Sub-Mariner segment. His design is the classic one, with him wearing a purple mask.
The first episode of the Iron Man show to feature the Mandarin was titled "The Death of Tony Stark". In this story, the Mandarin uses an orbiting satellite to shoot a death ray towards Tony Stark's mansion. As Iron Man, Tony manages to escape in time, but the Mandarin believes he has killed Stark. Iron Man then deduces who was behind the attack and travels to the Orient to confront the villain. Once there he learns the Mandarin was ready for him - a series of traps are waiting for him, but he manages to escape from all of them until he comes face to face with his arch-enemy. The Mandarin uses a paralyzing ray to render Iron Man helpless for a while, and plans on using his karate skills to finish him off. Iron Man however awakens earlier than the villain expected, but is still weakened. Trying to escape, the armored avenger finds a giant robot controlled by the Mandarin blocking his way out.
The next trap the Mandarin has come up with is tying Iron Man to a wheel, which will spin faster and faster until he is out of breath. But before activating the trap the villain reveals his origin to Iron Man, and explains his plan: to supply every country in the world with his test missiles, resulting in mutual destruction and him rising as ruler of the world. He has already given such a missile to the Chinese army, who don't waste any time to launch it. Iron Man manages to escape from the Mandarin's trap, and tries stopping the missile but only re-directs it (he sends it back to the place it was launched from). He confronts the Mandarin again, and manages to endure and survive the energy blasts his power rings. The battle ends when the Chinese army, angry at the Mandarin for what happened with the missile he gave them stat chasing after him, allowing Iron Man a chance to escape.
He returns in the next episode, "Ultimo". This time he has built a machine which allows him to find and transport Iron Man back to his lair. Though since he is unable to locate the armored avenger, Tony Stark (who was carrying the armor in his attache case) becomes his new target. This was back when Iron Man still had a secret identity so the villain had no way of knowing his machine actually brought him the person he wanted in the first place. Mandarin reveals his newest creation, the giant robot called Ultimo, which he built inside a volcano. The robot appears to be unstoppable, as it starts attacking the Chinese troops that surrounded the Mandarin's castle, wishing to conquer it. Thinking Stark is no longer of any use to him, the Mandarin blasts him with his power rings, throwing him into the castle's moat. Stark manages to suit-up with his armor, and goes ahead and confronts Ultimo.
For most of the episode, Iron Man seems to be out-matched by the Mandarin's robot. In a desperate attempt to escape, Iron Man lures Ultimo back to the volcano where he was created. The robot tries shooting his eye-beams at his prey, but accidentally hits the volcano, which erupts - and destroys Ultimo in the process as well. The episode also features at the beginning a short scene with an army general entering the Mandarin's castle, asking him to join his troops in the war. However Mandarin chases him away, claiming that he serves no nation and joining forces with someone would be beneath him.
In "The Mandarin's Revenge", Tony Stark as Iron Man investigates the disappearance of several missiles Stark has supplied the army with. Realizing the Mandarin is behind all of this, he travels to the Orient where he confronts the villain again, and once again manages to escape from all of his traps. The Mandarin asks Iron Man to join him, as his slave and they shall rule the world together, but the latter obviously refuses. He soon discovers just how the Mandarin managed to steal the missiles: with an interceptor ray that could change the trajectory of the rockets and bring them to his castle. Seeing Mandarin try to add another such rocket to his collection, Iron Man flies away and manages to save the rocket in time, but he is trapped by the Mandarin's ray and is brought back to the citadel.
This time the villain has prepared a hall of mirrors to confuse Iron Man, seeing as he has no way of finding out which is the real Mandarin and which are only reflections. The armored avenger manages to escape through a tunnel, and uses the control room to launch all the missiles Mandarin has stolen, sending them back to where they came from. Mandarin plans on using his interceptor ray again, but finds his weapon destroyed, with a note from Iron Man simply saying "Better luck next time, Mandy".
His final appearance on these Iron Man segments is in the episode "The Other Iron Man". When Tony Stark suffers a heart attack due to stress and is stuck in a hospital, his chauffeur Happy Hogan finds out he was Iron Man all along and plans on wearing the armor until his boss recovers. The Mandarin believes Happy is the real Iron Man and uses one of his machines to transport him to his stronghold. A weakened Tony Stark realizes what happened and wants to save his friend - but first stops by his factory to build himself another armor, more powerful and invincible than the previous model (although I thought it looked pretty much the same as the old one). He travels to the Orient where he manages to avoid the Mandarin's traps and rescue Happy, and also re-direct a test missile that was being launched from a Chinese base to hit the Mandarin's palace. Iron Man escapes just before the explosion, hoping that he saw the last of the Mandarin.
The Mandarin also has a short cameo in the final episode of the Namor the Sub-Mariner segments, titled "Doctor Doom's Day", an episode which guest-starred the X-Men (although oddly calling themselves the "Allies for Peace"), instead of the Fantastic Four. Mandarin is one of the many villains sent by Doctor Doom to attack the city, but he is quickly defeated by Cyclops' optic blast.
All in all, the Mandarin's first animated appearances were pretty good - the stories are more or less faithful adaptations of the classic comics, and I find them entertaining enough.