- Joaquin Phoenix as Larry "Doc" Sportello
- Josh Brolin as Lieutenant Christian F. "Bigfoot" Bjornsen
- Owen Wilson as Coy Harlingen
- Katherine Waterston as Shasta Fay Hepworth
- Reese Witherspoon as Deputy District Attorney Penny Kimball
- Benicio del Toro as Sauncho Smilax, Esq.
- Jena Malone as Hope Harlingen
- Joanna Newsom as Sortilège, who is also the narrator
- Jordan Christian Hearn as Denis
- Hong Chau as Jade
- Jeannie Berlin as Aunt Reet
- Maya Rudolph as Petunia Leeway
- Michael Kenneth Williams as Tariq Khalil
- Michelle Sinclair as Clancy Charlock
- Martin Short as Dr. Rudy Blatnoyd, D.D.S.
- Sasha Pieterse as Japonica Fenway
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- Martin Donovan as Crocker Fenway
- Eric Roberts as Michael Z. "Mickey" Wolfmann
- Jillian Bell as Chlorinda
- Serena Scott Thomas as Sloane Wolfmann
- Yvette Yates as Luz
- Andrew Simpson as Riggs Warbling
- Jefferson Mays as Dr. Threeply, Chryskylodon Institute
- Keith Jardine as Puck Beaverton
- Peter McRobbie as Adrian Prussia
- Sam Jaeger as FBI Agent Flatweed
- Timothy Simons as FBI Agent Borderline
- Samantha Lemole as Golden Fang Mother
- Madison Leisle as Golden Fang Daughter
- Matt Doyle as Golden Fang Father
- Liam Van Joosten as Golden Fang Son
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