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- Emma Thompson as Nanny McPhee
- Colin Firth as Cedric Brown
- Kelly Macdonald as Evangeline
- Derek Jacobi as Mr. Wheen
- Christopher Lee as Mr. Jowls
- Zoë Wanamaker as Selma Quickly
- Imelda Staunton as Mrs. Blatherwick
- Freddie Highmore as Simon Brown
- Angela Lansbury as Aunt Adelaide