- Ivana Baquero as Ofelia / Princess Moanna, a child who comes to believe she is the reincarnation of a princess from the underworld. Del Toro said he was nervous about casting the lead role, and that finding the 10-year-old Spanish actress was purely accidental. (The film was shot from June–October 2005, when she was 11.) "The character I wrote was initially younger, about 8 or 9, and Ivana came in and she was a little older than the character, with this curly hair which I never imagined the girl having. But I loved her first reading, my wife was crying and the camera woman was crying after her reading and I knew hands down Ivana was the best actress that had shown up, yet I knew that I needed to change the screenplay to accommodate her age."[11] Baquero says that Del Toro sent her many comics and fairy tales to help her "get more into the atmosphere of Ofelia and more into what she felt". She says she thought the film was "marvelous", and that "at the same time it can bring you pain, and sadness, and scariness, and happiness".[6]
- Sergi López as Captain Vidal, Ofelia's new stepfather and a Falange officer. Del Toro met with López in Barcelona, a year and a half before filming began, to ask him to play Vidal. In parts of Spain, López was considered a melodramatic or comedic actor, and the Madrid-based producers told del Toro, "You should be very careful because you don't know about these things because you're Mexican, but this guy is not going to be able to deliver the performance"; del Toro replied "Well, it's not that I don't know, it's that I don't care".[12] Of his character, López said: "He is the most evil character I've ever played in my career. It is impossible to improve upon it; the character is so solid and so well written. Vidal is deranged, a psychopath who is impossible to defend. Even though his father's personality marked his existence—and is certainly one of the reasons for his mental disorder—that cannot be an excuse. It would seem to be very cynical to use that to justify or explain his cruel and cowardly acts. I think it is great that the film does not consider any justification of fascism."
- Maribel Verdú as Mercedes, Vidal's housekeeper. Del Toro selected Verdú to play the compassionate revolutionary because he "saw a sadness in her which he thought would be perfect for the part".[12]
- Doug Jones as the Faun and the Pale Man. As the Faun, Jones guides Ofelia to the fantasy world. As the Pale Man, he plays a grotesque monster with an appetite for children. Jones had previously worked with del Toro on Mimic and Hellboy, and said the director sent him an email saying, "You must be in this film. No one else can play this part but you." Jones responded enthusiastically to an English translation of the script, but then found out the film was in Spanish, which he did not speak. Jones says he was "terrified" and del Toro suggested learning the script phonetically, but Jones rejected this, preferring to learn the words himself. He said, "I really, really buckled down and committed myself to learning that word for word and I got the pronunciation semi-right before I even went in," using the five hours a day he spent getting the costume and make-up on to practice the words.[13] Del Toro later decided to dub Jones with the voice of Pablo Adán, "an authoritative theatre actor", but Jones's efforts remained valuable because the voice actor was able to match his delivery with Jones's mouth movements.[14] Jones's dual casting is intended to suggest that the Pale Man (along with the toad) is either a creation of the Faun[15] or the Faun himself in another form.[16]
- Ariadna Gil as Carmen / Queen of the Underworld, Ofelia's mother and Vidal's wife.
- Álex Angulo as Doctor Ferreiro, a doctor in the service of Vidal, but an anti-Francoist.
- Manolo Solo as Garcés, one of Vidal's lieutenants.
- César Vea as Serrano, one of Vidal's lieutenants.
- Roger Casamajor as Pedro, Mercedes' brother and one of the rebels.
- Federico Luppi as King of the Underworld, Ofelia's father.
- Pablo Adán as Narrator / Voice of Faun.
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