Psilosynine was a neurotransmitter and one of the main chemicals involved in Betazoid telepathy.

In 2370, Lwaxana Troi suffered from low levels of psilosynine after prolonged telepathic communication with the Cairn. (TNG: "Dark Page")

Later the same year, Counselor Deanna Troi showed heightened levels of the chemical after experiencing a telepathic 'echo' in nacelle control. Dr. Beverly Crusher later gave her an inhibitor to suppress the levels of psilosynine, allowing Troi to enter the control room without being overwhelmed. (TNG: "Eye of the Beholder")

Psilocybin is a hallucinogenic alkaloid found in so-called "magic mushrooms", of the genus Psilocybe. It is likely that the writers of Star Trek chose the name to reflect the similarity.
In ultimately unused dialogue from the second draft script of DS9: "Accession", Dr. Julian Bashir explained about psilosynine, "It's a neurotransmitter involved in psychic phenomenon [sic]. We all have a little of it, but people who've been exposed to things like... Vulcan mind melds... the Bajoran orbs, are often left with more."

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