Cross-platform .NET/Mono bindings for LibVLC
My first guess was codecs aswell. .MKV is just a container that contains video and audio that are both encoded separately. Try playing your video files with the VLC Media Player from VideoLan, and while playing press CTRL+J to view all the codes info for that specific file. Maybe you find something useful when comparing the information of the videos that do work and those that don't.
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