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After filming the promo to Carmensita at Devendra's Los Angeles home over Easter weekend, the folk rocker has accompanied Natalie to the Big Apple, where she is currently filming her new movie New York, I Love You.
The couple have been spotted kissing and holding hands while walking in the trendy West Village area of Manhattan.
Natalie Portman and Devendra Banhart have reportedly split up.'The Other Boleyn Girl' star - who first started dating the folk singer in March after starring in the music video for his single 'Carmensita' - has decided to call time of their relationship, despite moving from New York to Los Angeles to be with Devendra.
A source close to the musician told In Touch Weekly magazine: "Natalie and Devendra have broken up.
Natalie Portman dated Devendra Banhart for 6 months.
Natalie Portman is currently married to Benjamin Millepied.
They met when she starred in Banhart's "Carmensita" music video, as his love interest, in March 2008.
They will remain friends but need some space and time away."In April, Natalie, 27, and the bearded singer, who is also 27, were photographed kissing and holding hands as they strolled through the West Village wearing matching black coats and sunglasses.
Natalie - who has previously been romantically linked to a host of actors including Jake Gyllenhaal, Zach Braff and Gael Garcia Bernal - recently vowed to never marry.