He's got the voice, and the build for it. You may never see his face, but I think Jeffrey Dean Morgan could handle it.
Runner Up: Karl Urban
The starship AI that won the hearts of geeks everywhere, should be played by an actress that has done the same. Feisty and intelligent while also being vulnerable, it was a match made in heaven. Plus, if made right we'll get to see a weird CG body scan naked version of Evangeline as Cortana.
Gunnery Seargent Buck
Why mess with a good thing. Let's include ODST Buck in the mox and cast the man who played him in Halo 3: ODST.
Michael 'Mickey' Crespo and the voice of the grunts.
Alan Tudyk voiced marines in the origianl games and Mickey in ODST. I say bring him into the movie and also have him work a little over time providing voices for a grunt or two. His range is so diverse he could do double duty and no one would notice.
Sergeant Major Avery Johnson
The stogy smoking Sergeant Major is at the frontline of almost every major battle in Halo, and Elba has displayed the tenacity and sarcastic timing necessary to play the bad ass that gives Master Chief his marching orders.
If you can't tell by now, I want a Halo movie to be a blance between ODST and Halo. ODST had dynamic characters that I'd love to see again, and the casting as spot on, so why not? Let's include geek favorite Adam Baldwin as his ODST Marine, Dutch.
Commander Miranda Keyes
The Commander of the ship "In Amber Clad" Keyes is pivotal in the fight against the covenant. She's intimidating and commands respect.
Runner Up: Katee Sackhoff
The Prophet of Regret
The chameleon actor would be perfect to play the Prophet that tries to lead the covenant on a suicide mission into another universe by activating all of the Halos. Serkis ability to shine through, even when he's not technically on screen makes him perfect.
ONI Agent Dare
Again, why change what worked, and the voice cast of Halo 3: ODST worked. Helfer as Dare was perfect and her chemistry with Fillion was amazing.
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