iTunes movies are DRM'd, so no they wont work.



Good luck finding a way to get non-DRM'd video content, you can't even pay for it these days.

Your best bet will be ripping DVD's (they are DRM'd as well, but with a well known weaker and easy to break encryption) However you should be warned that this may be illegal if you live in a jurisdiction that attempts to prop up failed technical restrictions with legal cruft (i.e. in the US the DMCA makes nearly *any* type of DRM circumvention illegal, even schemes as weak as that on DVD's)