How can I save some music locally and the rest to an external drive or NAS?

I love my MBP w/ 16 GB RAM and SSD drive EXCEPT ... the SSD drive is lacking storage.
I'm trying to find a way to store select songs/photos/videos locally and the rest on an external drive or better yet a NAS, while still getting the convenient use of iPhoto and iTunes.  Ideally, I would configure certain albums/playlists to stay local while the full library of media is on the external storage and when I plug in my iPhone/iPad the new photos/videos would upload to the external storage.
Has anyone discovered a way to do this?
Do I need to consider other programs like Lightroom to pull this off?

Setting it up the way you have with the library on the internal and just the media on the external makes it a lot more tricky to move things around. If it was all on the external you could do in the time it takes to copy the files plus about 20 seconds.
You can use the same library file, except in that file are references pointing to the media files on the USB drive.  Are you planning on doing this with the same USB drive that you are using right now>?  It is possible it may work.  If the configuration is that you have SongA on USB drive Fred, as long as the drive remains named Fred then you should be able to move it to a different point of attachment.  If you are planning on using a different USb drive you can try renaming the new USB drive to the exact same name as the existing one and maybe trick iTunes into not noticing the difference.
This is where having as much detail as possible when posting an issue is helpful so we don't have to consider every possible configuration.

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