Viggo was first introduced to Buckethead's work while working on sounds for an educational CD on Greek mythology.The finished product included a guitar part by Buckethead, which caught Viggo's ear and led him to initiate contact with the guitarist. Mortensen is featured on The Lord of the Rings: The Return of the King soundtrack, singing "Aragorn's Coronation" (the name of the extended version of this song in the 3rd original sound track is "The Return of the King"), the words by Tolkien and the music composed by Mortensen.His mother was American, while his father was Danish; they met in Norway.

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Mortensen experiments with his poetry and music by mixing the two art forms.

He has collaborated with guitarist Buckethead on several albums, mostly released on his own label (Perceval Press) or TDRS Music.

Other well-received films have included Appaloosa (2008) and Far from Men (2014).

He received a second Best Actor nomination in 2017 at the 89th Academy Awards for his role in Captain Fantastic.

In the extended DVD edition of the first Lord of the Rings movie, The Fellowship of the Ring, he sings the song "The Lay of Beren and LĂșthien".

His poems are written in English, Danish, and Spanish.

In 2005, Mortensen starred in David Cronenberg's movie A History of Violence as a family man revealed to have had an unsavory previous career.

He was nominated for a Satellite Award for Outstanding Actor in a Motion Picture for this role.

Aside from acting, Mortensen's other artistic pursuits include fine arts, photography, poetry, and music.