Limewire is a file sharing program with a crummy media player attached to it. iTunes is a media player with a (crummy?) online store attached to it. So really, they are two different applications.
You need iTunes to put music on to an iPod (there are other options, but I havn't seen any better then iTunes on the Mac platform). So really, you are looking to get music in formats that iTunes can handle, which is pretty much everything excluding protected music from outside the iTunes store.
Using something like LimeWire, you can find mp3 encoded files that can be imported into iTunes and then loaded into your iPod. However, not sure the mods around here will want people talking about how to pirate music.
Your best bet is to "rip" your CD collection onto your Mac using iTunes, and then sync the iPod to it. Default settings work fine, but you might want to play around with them to up the quality (I use 256kbits). Also, if you want to move your music collection to a different media manager then iTunes, rip them as MP3's rather then the Apple format.
Given the amount of garbage flying around on Limewire, I'd advise you to stay away from it and stick to legal torrent sites or direct artist releases.
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