Too be honest, I don't think FLCL should ever be made into a live-action movie. Stemming from Lord Canti, to Amarao's eyebrows. It just wouldn't work. But its always fun to fancast.
DIRECTOR/PRODUCER
As for director, I'm going with David Fincher. He'd easily be able to transfer the tone of the anime. I don't exactly know about his visual abilities, and the anime is heavy on their visuals. So I'm going with Brad Bird as producer. If an FLCL movie ever happens, heres to hoping.
JOEL COURTNEY as NAOTA NANDABA
This was a tough choice. There are a lot of child actors, but few who could possess Naota's angst and anger. Courtney is one of the few who I think could.
LINDY BOOTH as HARUKO HARUHARA
This one was no contest. Booth looks the part down to a T, and could probably possess the spontaneity and pure lunacy that is Haruko.
ELLEN PAGE as MAMIMI SAMEJIMA
Probably the hardest one. She looks like Mamimi enough, or at least could. She's also not terrible at serious roles.
MATTHEW FOX as COMMANDER AMARAO
Honestly, I couldn't think of another actor who could do it as well as him. Hes perfect for the serious guy who you don't want to take seriously. As for the eyebrows, CGI exists for a reason.
SELENA GOMEZ as LIEUTENANT KITSURUBAMI
Another hard one. It was between her and Michelle Rodriguez. But I think Selena Gomez possesses the younger and more mature qualities needed.
ELLE FANNING as ERI NINAMORI
Dye her hair black, give her glasses, and you have Ninamori.