Officers lashed out against Kate and Gerry McCann's slick PR operation after learning they had granted an interview to glossy magazine Vanity Fair, and could even make £2million from a film about their daughter's disappearance.
A source close to the investigation said detectives were furious about the latest publicity, which came as formal requests for the McCanns' friends to be reinterviewed were sent to Britain.
The attacks are a clear indication of the anger that the McCanns' publicity campaign has caused in Portugal, where police investigations are usually carried out in secret.
They came as Gerry McCann revealed he is tortured by guilt that Madeleine's disappearance is his fault.
In an interview with Vanity Fair, he also admitted there was only a "slim" chance his daughter was alive - the closest he has come to conceding the fact.
"I wish I hadn't gone to the tapas bar," Mr McCann told the society magazine. "I wish I'd stayed in the apartment that night. I wish I'd stayed in the room when I checked on her five minutes longer. Of course we feel guilty about not having been there and that is just something we have to deal with for the rest of our lives. We live this 24 hours a day."
Mr McCann, 39, gave the interview alone in October, without his wife Kate, after being approached by the magazine.
Vanity Fair also spoke to the couple's friends and family as well as to the other suspect in the case, Robert Murat.
Mr McCann's sister Philomena told the magazine that he had called her on the night Madeleine vanished and sobbed: "It's all my fault, because Kate and I went out to dinner."
Clarence Mitchell, the family's spokesman, said Mr McCann had not been paid by Vanity Fair and had instead requested donations to the fund in return for cooperation with future projects.