The three men and two women, aged between 29 and 45, are, the CPS says, accused of "conspiring to collect information intended to be directly or indirectly useful to an enemy".
Orlin Roussev, 45, from Great Yarmouth, and Bizer Dzhambazov, 41, and Katrin Ivanova, 31, both from Harrow, west London, will appear in Westminster magistrates court on 26 September for an initial hearing.
They will be joined by Ivan Stoyanov, 31, from Greenford, west London, and Vanya Gaberova, 29, from Churchway, north-west London. All five have been charged with offences contrary to section 1 of the Criminal Law Act 1977.
Roussev, Dzhambazov and Ivanova were previously charged with "possession of false identity documents with improper intention" in February, news of which emerged in August.
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