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Berzerk: Ports of the Stern coin op classic Berzerk appeared on Atari's 2600 VCS and then later on the 5200 Supersystem in a version that actually has speech. The VCS version has simplistic graphics and no Otto, but is still an immensely fun game. I played it for hours just to see all the different colors of Robots.
Star Raiders: I never owned this title until after I had played the version that existed for my Atari 800 (which is an exact copy of the Atari 5200 Star Raiders). I loved this game a tremendous amount, but I found the VCS version to be much better. It was one of the games to come packaged with a keypad controller and overlay, which used the second joystick port. You controlled your shields, computer, and warp drive with this and steered and fired you guns with the joystick. The "tuning fork" crosshairs still sits in my mind! I love this game, and you should too. The keypad controllers were packed in with the game, and it's pretty common. You should be able to find a Star Raiders cart and a keypad controller at a local thrift, but the overlays are slightly harder to find.
Asteroids: A classic VCS title. I spent hours chasing the flickering rocks as they didn't tumble through space. Incredibly simplistic and very fun.
Defender: Another coin-op port which really shouldn't have been, IMO. The ColecoVision shined in the coin-op conversion scene whereas Atari really couldn't due to the severe limitations of its VCS system. This game flickers, is hard to play, and is just not fun. This didn't stop it selling huge amounts of carts, though, so it's one of the most common.
Space Invaders: This is a title where the graphics simply don't matter. It's addicting, fun, and above all, just great. This is a get-your-friends around the TV game and play it for hours. Interestingly enough, this game appeared post crash as well, and is one of the few carts to have FOUR major label variations.
Yars' Revenge: Apart from being one of the most awesome titles for the VCS, all I can really say is that this game took incredible amounts of imagination and hemp to design.
Adventure: One of the BEST VCS titles, period. Simplistic graphics, simplistic music, simplistic ideas. Find the chalice and bring it back to the castle. You have to use a variety of objects like a magnet, a wall-bridge and a sword to avoid dragons and other stuff. The maze is hard to get through and is very challenging. Damn bats!. I love this game, and you should too.
Indy 500: This game featured a special paddle-like controller called the Racing Controller which spun forever in each direction, allowing you to better turn. This game is a lot of fun. The racing controllers can be modified to play Tempest 2000 on your Atari Jaguar the way it should be played.
Night Driver: You used the paddle controllers to maneuver your car along the windy road. Graphics aren't that great, but the gameplay is.
Bowling: The gameplay of this title is almost comical, but since my mother bought it for me back in the day, I still like it. It compares nothing to real bowling. :)
Golf: Proof that sports titles were best left to Mattel.
Video Olympics: Atari did pretty well during the 1970's making pong consoles and pong machines, so it's only fitting that they made several carts for the VCS that had pong themes. Video Olympics is an entertaining collection of variations of pong that are fun with two people. Still doesn't beat an Atari Super Pong console though.