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Published 18:32 29 Sept 2016 BST
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It means the FA have now been forced to find a replacement - and the Telegraph's Matt Law reports that they are ready to speak to Rangnick about the role.
It will be the second time they have interviewed the German 58-year-old after they held talks with him in the summer, before opting for an English boss in Allardyce.
But the former Hoffenheim and Schalke boss is said to have impressed FA technical director Dan Ashworth, chief executive Martin Glenn and vice-chairman David Gill.
Indeed, former West Brom director of football Ashworth has long been an advocate of Rangnick, having previously attempted to take him to the Baggies as manager.
He is currently the director of sports at Bundesliga club RB Leipzig - but that hasn't stopped someone editing his Wikipedia page...
Under 21s boss Gareth Southgate will take charge of the senior team for the next three World Cup qualifiers, and the friendly against Spain, while the process of appointing a full time successor for Allardyce is completed.
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