The singer - known for her eccentric performances and dress sense - posted an updated set of lyrics to her song Declare Independence on her Facebook page.
The new lyrics say: "Scotland! Scotland! Scotland! Declare independence! Don't let them do that to you!"
The rest of the lyrics are those of the original song, including the lines: "Start your own currency! Make your own stamp. Protect your language" and "Damn colonists. Ignore their patronizing. Tear off their blindfolds. Open their eyes."
The original Declare Independence song was written to call for independence for the Faroe Islands and Greenland, which are both ruled by Denmark, as Björk's home country of Iceland had been before it became a sovereign state in 1918.
It's not the first time Björk has re-appropriated the song: a dedication to the troubled region of Kosovo in 2008 led to a Serbian festival gig being cancelled.
Reaction to the post was mixed on Björk's Facebook page. One unimpressed poster said: "Politics aside. Those lyrics are shite," and others lambasted her for "wheeling out a old song to get publicity".
But others said the post was another reason to admire "the brilliance that is Björk". One commenter said simply: "Thank you Bjork!! VOTE YES!!"
The original military-themed performance video for Declare Independence can be seen below: