Help to use Cruzer Glide 64GB to transfer Itunes folder?

Do you mean if any of the files individually inside the folder are larger than 4GB?

Will I not be able to transfer my itunes folder unless I do this?

No, I mean if, for example, your folder contains 100 itunes and  2 of them are each larger than 4 GB those 2 files will not fit but the others will.  If you look at the files in your iTunes folder using Windows Explorer you can see how big they each are.   Are any over 4,000,000 KB?