How do I take songs off Ipod Classic if they are no longer in ITunes?

I've nearly filled my Ipod Classic with music. Since my computer only has so much storage and ITunes couldn't possibly store all the songs, I kept deleting them, then would add new ones, move them manually to the Ipod, and then delete them. I continued this cycle to get as much music as I wanted on the Ipod. But now I'd like to add some new music and I'm willing to sacrifice some of the music that's on the Ipod. So how do I remove songs from the Ipod if they are no longer in ITunes?

It sounds like your iPod is set to use the Manually manage music and videos setting, which is on the iPod's Summary screen in iTunes.  When you use the manual method, the iTunes library on the computer is not linked in any way to the library on the iPod.
So how do I remove songs from the Ipod if they are no longer in ITunes?
So, that does not even matter.  iTunes is not keeping the two libraries "in sync" in any way.  First, if the iTunes sidebar (along left side of window) is hidden, from the menu bar, under View, select Show Sidebar.  The iPod appears in the sidebar, under DEVICES, when connected.
To remove songs from the iPod manually, click the small triangle to the left of the iPod's name (in the sidebar) to drop down its content list, indented below the iPod.  Click on Music there.  The list of songs on the iPod is shown to the right.  Select the song you want to remove and press Delete on the keyboard.  You can do this with more than one song selected.
NOTE:  It is a bad and risky idea to keep the only copy of song files on an iPod, which can become lost, broken, or in need of a Restore.  You will eventually lose your music.  You should keep all of your songs in your iTunes library on your computer (as the "master copy").  If the internal drive does not have the space, you should get an external drive that is large enough to hold all of your songs (with room to grow).  You can then set up iTunes to store its iTunes Media folder on the external drive. 
http://support.apple.com/kb/ht1449

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