Biser Dzhambazov, 41, Katrin Ivanova, 31, and Orlin Roussev, 45, were arrested by counter-terrorism police in February and charged with having fake identity documents with "improper intentions."
The trio were charged under the 1911 Official Secrets Act with the government alleging they worked for the Russian intelligence services, the BBC reported.
The trio had passports and documents from Spain, Italy, Croatia, France, the Czech Republic, Greece, and Slovenia, the report added.
The Metropolitan police said the three were arrested in February while two other people were arrested at the same time. All five are due in court in September with a trial set for January.
Ivanova and Dzhambazov are believed to be a couple and have lived in Britain for about a decade and ran an organization to help integrate Bulgarian immigrants into British society.
The pair reportedly assisted the Bulgarian election commission's process of expatriate voting in Britain.
Roussev moved to Britain in 2009 and has business ties to Russia, the BBC said.
Roussev has been described as a software engineer and claims to have worked for the Bulgarian Energy Ministry and to have owned the now-defunct company NewGenTech Ltd.
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