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Then just choose "Activate a product on Steam", and you should be able to enter your CD-key. :)
This is a list of retail games that can be activated on Steam. If it's not on there, I'm afraid we can't help you.
Add a Game -> Add a Non-Steam Game
Locate the executable and add it, you can rename the 'Sims3Launcher' (or whatever it was by default) to 'The Sims 3' when you right mouse click it and go to Properties on the Steam -client.
The reason the CD-key doesn't work, is because Sims isn't a Steamworks - title. The only way it goes through the Steam -client is if it's bought from the Steam Store directly, and only then do the DLCs from Steam Store work with the basegame.