Staff at the Sea Life centre in Oberhausen said they were devastated to learn that he had passed away during the night.
Paul made his name by successfully choosing a mussel from one of two boxes bearing the flags of competing nations.
Octopuses rarely live beyond two years so his death was not unexpected.
Paul was two-and-a-half years old and had been hatched at another centre at Weymouth in England in 2008.
So farewell… Paul the octopus, famous for predicting football results.