Police swooped on a series of homes in Plymouth after officers uncovered a cache of weapons, suspicious devices and suspected extremist material during a search.
The three men and two women were held under the Terrorism Act over the last three days, Devon and Cornwall Police said.
They are being questioned over claims they planned to target the meeting of the world's most powerful political leaders in London later this week.
Scotland Yard officers are liaising with investigators in south west England over the suspected plot.
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