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Michael Sheen as Aziraphale, an angel who has lived on Earth since the dawn of creation. He guarded the East gate entrance to the Garden of Eden with a flaming sword, which he gave to Adam and Eve on their expulsion from the Garden out of concern for their well-being. He has grown to love the finer things of human life, enjoys haute cuisine and owns an antiquarian bookshop in London.
David Tennant as Crowley, a demon who has lived on Earth since the dawn of creation. Originally called "Crawly", he is the Serpent who tempted Eve with the apple from the tree of knowledge of good and evil.
Sam Taylor Buck as Adam Young (series 1; guest series 3), the reluctant Antichrist accidentally placed in the custody of the Young family.
Jon Hamm as Gabriel (series 1–2), the leader of the forces of Heaven. While Gabriel was only mentioned once in the original novel, his role was meant to be expanded in the unfinished sequel to Good Omens; Gaiman incorporated parts of the planned sequel into the TV series's plot. In the novel, the leader of the forces of Heaven was the Metatron.
Daniel Mays as Arthur Young (series 1), father of Adam
Siân Brooke as Deirdre Young (series 1), mother of Adam
Ned Dennehy as Hastur (series 1), a demon
Ariyon Bakare as Ligur (series 1), a demon
Nick Offerman as Thaddeus Dowling (series 1), the US Ambassador to the UK and father of Warlock
Anna Maxwell Martin (series 1) and Shelley Conn (series 2) as Beelzebub, the leader of the forces of Hell. Though portrayed by women, Gaiman has said the show's version of Beelzebub has no pronouns.
Nina Sosanya as:
Sister Mary Loquacious (series 1), a nun of the Chattering Order of St. Beryl, a satanic order of nuns who had to switch a human baby with the Antichrist. After the convent burns down, she becomes manager of the business management centre established on the same site.
Nina (series 2), the owner of the coffee shop "Give Me Coffee or Give Me Death" which is across the street from Aziraphale's bookshop
Maggie Service as:
Sister Theresa Garrulous (series 1), a nun of the Chattering Order of St. Beryl
Maggie (series 2), Aziraphale's tenant and a record shop owner
Doon Mackichan as Michael, an archangel
Frances McDormand (narrator, series 1; guest series 2) and Tanya Moodie (series 3) as God
Adria Arjona as Anathema Device (series 1), Agnes Nutter's last descendant and an occultist who eventually teams up with Newton Pulsifer to try to stop the end of the world
Miranda Richardson as:
Madame Tracy (series 1), a part-time medium and courtesan
Shax (series 2), a demon and confidante of Crowley's
Michael McKean as Witchfinder Sergeant Shadwell (series 1), the last officer of the once-proud witchfinder army
Jack Whitehall as:
Newton Pulsifer (series 1), a struggling computer engineer and descendant of witchfinder "Thou-Shalt-Not-Commit-Adultery" Pulsifer
"Thou-Shalt-Not-Commit-Adultery" Pulsifer (series 1), the witchfinder who burned Agnes Nutter at the stake
Mireille Enos as War (series 1), one of the Four Horsemen of the Apocalypse that appears in the form of war correspondent Carmine "Red" Zingiber
Bill Paterson as R. P. Tyler (series 1), a member of the Tadfield Neighbourhood Watch and neighbour of the Young family
Yusuf Gatewood as Famine (series 1), one of the Four Horsemen of the Apocalypse who appears in the form of dietician and entrepreneur Raven Sable
Lourdes Faberes as Pollution (series 1), one of the Four Horsemen of the Apocalypse and appears in the place of Pestilence who has retired as a Horseman upon the discovery of penicillin
Brian Cox (voice) and Jamie Hill (body) as Death (series 1), one of the Four Horsemen of the Apocalypse
Gloria Obianyo as Uriel (series 2–3; guest series 1), an Archangel
Liz Carr as Saraqael (series 2–3), an Archangel
Quelin Sepulveda as Muriel (series 2–3), an angel
Actors credited in the opening titles of episodes in which they play a significant role.
Reece Shearsmith as:
William Shakespeare (series 1)
Furfur, a demon official (series 2)
Mark Gatiss as Harmony (series 1–2), a Nazi agent whom Aziraphale and Crowley encounter during the London Blitz
Steve Pemberton as Glozier (series 1–2), a Nazi agent and Harmony's partner
Niamh Walsh as Greta Kleinschmidt (series 1–2), a Nazi double agent
David Morrissey as Captain Vincent (series 1), the captain of the cruise ship that runs aground on Atlantis
Simon Merrells as Leslie the International Express Man (series 1), a man who helps summon the Four Horsemen of the Apocalypse
Derek Jacobi as Metatron, the spokesperson for God
Johnny Vegas as Ron Ormerod (series 1)
Andy Hamilton as the voice of Hell's Usher (series 1)
Benedict Cumberbatch (voice) and Niall Greig (performance capture) (series 1) and Toby Jones (series 3) as Satan, the ruler of Hell
Elizabeth Berrington as Dagon (series 2; guest series 1, 3), one of the elite demons in Hell
Peter Davison as Job (series 2)
Andi Osho as Sitis (series 2), Job's wife
Ty Tennant as Ennon (series 2), son of Job
Sean Biggerstaff as Mr. Dalrymple (series 2), a doctor in 19th-century Edinburgh
Julie McLellan as Wee Morag (series 2), a poor woman in 19th-century Edinburgh
Abigail Lawrie as Elspeth (series 2), a poor grave-robber
Tim Downie as Mr Brown (series 2), a carpet salesman and chair of the Whickber Street Traders and Shopkeepers' Association
Donna Preston as Mrs Sandwich (series 2; guest series 3), a seamstress/brothel owner on Whickber Street
Siân Phillips as Mrs. Henderson (series 2), a 1940s cabaret impresario
Pete Firman as Pat (series 2), the proprietor of a magic shop in the 1940s
Paul Chahidi as Sandalphon (series 3; guest series 1), an Archangel
Bilal Hasna as Jesus (series 3), the "Son of God" who is to return to Earth as part of the Second Coming.
Sean Pertwee as Brian Cameron (series 3), a crime boss operating in Soho
Mark Addy as Harry the Fish (series 3), a card player who befriends Jesus