After all the experimenting I have done, I have come to the conclusion that the issue lies with the Apple TV.. NOT your computer..
First the symptoms:
1. ATV lists all videos, music, pictures etc. within the Library, including navigating to nested 'choices' accurately (for example, Computer->Movies->Drama->Movie).
2. All data for Library is displayed accurately - cover art, actor/director/producer info, summary etc. for two different libraries, one Windows, one OSX.
3. Videos - movies, tv shows, iTunesU do NOT play. ~5Min. spinning with a timeout claiming connection issues.
4. Music does play. No sign of 'connection issues'
Tried Fixes/Testing:
1. Reboot ATV - does NOT work.
2. Reboot Router - does NOT work.
3. Testing on mobile devices (3 iPhones, 1 iPad, 2 Minis) - DOES work for Home Sharing, streaming video for both libraries (Win, OSX).
4. Connect ATV to host with iTunes and 'rescue' - resolved all issues. (ATV IS THE ISSUE)
Apple TV displays the same issues frequently, but not in a given pattern, such as every 1-2 months (but close) - have been dealing with the issue for over a year. The only fix I have found its to connect a mini usb to the ATV, and plug in to the iTunes host for 10Min. to 'rescue'.
After the fix, everything is lightning fast, video load times etc., then slowly degrades to ~10-20sec. load time, plateaus and then eventually falls in to a 'no load' from the library state - and its 'rescue' time again..
...and its always when I REALLY want to watch a specific movie or show...