How can I delete something permanently from my itunes library?

Everytime I delete the media, when I re-sync it just appears again. I have some downloaded media that I want to permanently remove so that my children are not able to access it when we go to sharing after Christmas. Thanks!

Thank you gbeast. I have tried that several different ways. I think the problem is that I am trying to delete past purchases from the itunes store because they keep copying back to my phone during the re-sync. Do you possibly have a solution for this?

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