National Intelligence Organisation (MIT) has suspended 141 personnel in an internal probe over links to US-based preacher Fethullah Gulen who Ankara alleges was behind the coup.
Of these, 87 have now been expelled, the Anadolu news agency said. Criminal complaints have been lodged against 52 of them, it added.
In a separate development, Turkish police detained 41 suspects from a charity organisation Kimse Yok Mu? (Is There Anyone There?) for alleged links to Gulen, Anadolu news agency reported.
Turkey's secret service was widely criticised for not warning authorities about the coup bid and the government has acknowledged a vacuum in gathering intelligence.
The 87 staff from the Turkish intelligence will no longer be able to work in another state institution after their dismissal, Anadolu also reported.
There had been intense speculation over the future of Turkish spy chief Hakan Fidan after President Recep Tayyip Erdogan publicly said intelligence lapses had helped the coup.
Fidan was named to head MIT by the Turkish president in May 2010 after serving as his foreign policy adviser for three years.
Erdogan, who described Fidan as his "secret keeper", had made no secret of his discontent when the spy chief in February 2015 resigned as head of MIT with the aim of becoming an MP from the president's ruling party.
But later Fidan withdrew his candidacy and remained at the top of the intelligence service.
Several top ministers, including Foreign Minister Mevlut Cavusoglu, have grown facial hair in recent months in what is widely seen as a sign of loyalty to the moustachioed head of state.
The MIT is one of Turkey's most secretive but powerful organisations, handling issues ranging from internal security to the sensitive areas of foreign policy.
Turkish police carried out operations in 18 provinces including in the mega city Istanbul in search of 121 suspects linked to Kimse Yok Mu?, which had been shut down by authorities in the wake of the coup along with other Gulen-linked groups, Anadolu reported.
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