1) Through the files section, Remote Buddy will resolve *Finder* 
symbolic links (which are just files) for you and send the real path 
to VLC.

2) Through the movie library, Remote Buddy will send the VIDEO_TS 
directory path to VLC. If you were using Finder symbolic links (again, 
which are just files) and VLC can't detect and handle them, then 
you'll of course get errors as VLC will try to parse a special Finder 
file as movie file and that's prone to not work.

Solution: 
Use real filesystem-level symbolic links, not Finder link files. On 
the shell:

ln -s pathFromFile pathToDestinationOfLink

f.ex.

ln -s /Volumes/SomeOtherVolume/Movies/MyMovie.avi /Users/theuser/ 
Movies/MyMovie/VIDEO_TS/MyMovie.avi

It's probably easier to maintain and less time intensive to build the 
correct file structure in the first place, though, rather than working 
with links.

If you want VLC to support Finder link files, please contact the VLC 
team, as I'm not involved with the VLC project.

Best regards, 
Felix Schwarz