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In Photos, the equivalent to show photos that aren't in an Album, the Smart Album would have the conditions; "Album" "is not" "any".

For Music you would need; "Playlist" "is not" "any". As these conditions aren't listed, I'm guessing that it can't be done.
 
It seems like you could make a smart playlist with "playlist" "is not" <each of your existing playlists> and then stack up ALL of your playlists in that filter. For example, if you have 30 playlists, you'll have 30 entries that are all "playlist" "is not" referencing each playlist. Here for example would be a starter of building this by selecting 2 holiday playlists...

PlaylistExclusion.jpg

If I added the rest of my playlists like those 2, I'm guessing what would be left would be songs not in any of the my playlists.

I did a minimal test where I made a 1 row version of this and the total songs in this playlist was reduced by the number of songs in the filtered playlist. Then I added another "is not" rule for some songs still showing that I knew were in another playlist and those songs disappeared. Then I added another "is not" rule for some songs still showing that I knew were in another playlist and those songs disappeared. So, I believe if I put ALL of my playlists in this smart playlist, I'd end up with only songs not in any playlist. Based on this partial test, I'm about 90% confident this would work for OP.

OP, I suggest testing the above by checking song counts in a few of your playlists and then making just a one-line version of this smart playlist trying each "is not" playlist. For example, Playlist A has 1200 songs, B has 800. You know your "total songs" number. So try making this with A and total songs in this playlist should be total songs minus thoe 1200 songs. Now switch that to B and it should be total songs minus 800, etc.

If you KNOW for sure you have at least 2 playlists with no overlapping songs- that is, the same songs are not in both playlists, you could grow confidence in this method by putting one of the playlists in this filter to see total songs minus the number of songs in one playlist... then adding a new row and the second playlist to see the result being total songs minus playlist 1 and minus playlist 2. It won't take much of that kind of approach to realize that if you put ALL of your playlists in such a rule, it should result in a playlist of songs not in any of your playlists.

Shortcut option: create a temporary playlist that would basically be "All Songs in Playlists." Drag all songs from all of your playlists into this temp playlist. Now use the above "is not" option to filter this one playlist. That should eliminate all songs in all playlists by having to use only one "playlist" "is not" choice. Once you have the smart playlist result (of all songs not in any playlist), create a "NotInAnyPlaylist" (not smart) regular playlist and drag all of these songs into it. Then you can delete the smart playlist temp playlist you created to filter for this result AND the smart playlist "is not" playlist, eliminating the "one time use" clutter of both of those but leaving you with a net of one new regular playlist made up of only songs in no other playlist.

If that doesn't work- but I'm pretty confident it will- here's a few hack options...

If you don't have too many playlists, open each playlist and uncheck all. Then go to "songs" and those that remain checked are not in any playlist. Maybe put them in a "NotInAnyPlaylists" playlist then go back through your playlist and re-check all again.

Less reliable: if you regularly play your playlists, look through their songs for oldest "last played" date. Then in "Songs" sort by last played date. Everything before your oldest "last played" date is not in any playlist. This option will probably miss a few where you have played a few songs not in a playlist since that oldest "last played" date, but that would probably get most of them.

Another less reliable option if you regularly play your playlists: Play count should be higher than songs never played or rarely played. For example, if your playlists average is- say- 8 plays, I would guess play count numbers of 1 or 2 is probably songs not in any playlist.

In all of these you could then make a playlist of "NotInAPlaylist" and then you could eyeball your way through all of the songs in this playlist with right click, "show in playlist" to discover any that actually are in some playlist and manually delete them from this playlist. That would ultimately lead to a true "not in any playlist" playlist.
 
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