ITunes won't add large files to the library

I use software to convert my personal DVDs into Apple TV format via H.264 decoder for 720p resolution. The resulting files are typically larger than 3GB for a 2 hour movie. Now iTunes won't add them to my library so I can't sync them or stream them to my Apple TV.
Any advice? Is there a setting in iTunes that I overlooked?
I have tried the mpg4 conversion setting for 480 resolution and those files will load into iTunes and stream to Apple TV, but they are grainy and a horrible quality. So for those saying I don't need to use the H.264, I am picky and want a high quality resolution.
Thanks for any advice and help.

RPojeta wrote:
It is possible that there is something else wrong with my files. Several mp4 files worked fine prior to getting a new iMac and transferring the files over (using ext HDDs, not the migration wizard). Quicktime won't even open the files in question. It states that they are not movie files.
Sounds odd, they may be corrupted.
Try enusring the file extensions are either .mp4 or .m4v (or .mov perhaps).
3GB+ for a file intended for AppleTv 2 hours long sounds excessive and may exceed AppleTv playback specs but it shouldn'tbother quicktime. If the files don't open in QT they may well be corupted.

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