I'm not entirely sure, but you could try the following:

1. Delete your entire current library of music and movies, but do not send the 
files to the trash.

2. In preferences, in the advanced pane, select the new location you'd like to 
use for your iTunes Media library (e.g. an external disc).

3. Either
(a) Copy the Music and Movies folders from your iTunes Media Library folder to 
the Automatically Add to iTunes folder in the new iTunes Media folder on your 
external HD;
or
(b) Ensure the "copy music files to iTunes Media folder when adding to library" 
option in the advanced pane of iTunes preferences is checked, and then go to 
file > add to library, and add your old Music and Movies folders to your iTunes 
library.

4. Once you've re-added all your music and movies to iTunes by one of the 
methods in point 3 you could delete the Music and Movies folders from your old 
iTunes Media folder and then empty trash to free up space.

You should probably create a back up duplicate of your Mac before trying this 
in case it works out badly.

All the best and hope some of this helped.

Nic

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