There’s a professional video biography of Aleister Crowley available in 5 parts on YouTube – here. Despite a few attempts at balance, it strongly emphasizes the most shocking and depraved aspects of Crowley’s life and works. Unfortunately (or fortunately) there’s nothing about tarot in the film.
To get the other side, and perhaps erring on the side of sweetness, try this commentary featuring Lon Milo DuQuette – here.
Check out these art exhibits featuring the art of Aleister Crowley and Frieda Harris – here.
Frieda Harris’ alternate versions and sketches for the Thoth deck can be seen here. Harris’ use of Synthetic Projective Geometry and friendship with Olive Whicher is here. A bio of what little is known about Frieda Harris is here. (Note: Harris spent her most of her last years in India.)
A collection of the letters between Crowley and Harris regarding the creation of the Thoth deck are available here.
A feature film on Crowley written by musician Bruce Dickinson is scheduled to open this month. In this supernatural occult thriller, the spirit of Crowley possesses a modern Cambridge professor (Simon Callow). I don’t know if there is any tarot in it. See the trailer (which I’ve heard is better than the movie):
Added: the official website – here.
Hear Bruce Dickinson talk about making the film here.
Read a review of the film by Ivor Davies here (warning: spoilers): “This is the crux of the problem that this film has – just what would someone possessed by the late Aleister Crowley do all day long? ‘Sex and murder’ unfortunately is this film’s disturbing answer.”
An interesting article on how Crowley has been fictionalized in literature can be found here.