The force said Wednesday's raids involved 100 officers who made raids at 13 locations across the capital.
During the operation a total of 40,000 pounds (US$80,000) in cash was seized, as well as a variety of false passports, drivers' licenses and foreign identity documents, Metropolitan police said in statement.
"The production of false passports enables others to commit a range of serious crime," said lead officer Detective Chief Inspector John Kielty. "This operation tackles the criminals who try to hide their true identities from enforcement authorities."
Kielty described two of the raided properties as "sophisticated factories," which could produce a range of documents. He added that the majority of the individuals arrested said they were Brazilian.
Police say the street value of false passports ranges from 200 pounds to 5,000 pounds.
On Tuesday, Britain's Home Office said about 10,000 legitimate British passports were issued to fraudulent applicants last year.
Among those who were issued passports after making fraudulent claims are two convicted terrorists.
Dhiren Barot, now serving a 40-year sentence for conspiracy to murder, got two passports before he was arrested in 2004.
Salaheddine Benyaich, a Moroccan now imprisoned in his country for terrorist offenses, held two British passports in the name of a British citizen.
Thursday's operation was not linked to terrorism, police said.