How can I remove songs from my device without iTunes?

There was a time in iTunes that you could uncheck songs that you didn't want to sync to a device. When I connect my phone to my iTunes account, select the device and show the songs and playlists, at one time you could uncheck songs, resync the device and those unchecked songs wouldn't appear on the device. That capability doesn't seem to exist. Is there another way?

[Re-Titled by Moderator]