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You need to kill the big daddies, but you can choose to free the little sisters or convert them to pure Adam. There is no alternative method for Adam acquisition.

This is obviously where you collect the majority of the Adam in the game but there are other places for small amounts. I am not far but I know befor you enter sirens alley there is Adam in the shape of coral in the water. I think 3 of them for a small total of 30.

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Q: How do you get Adams on BioShock without any little sisters?
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