The NFS share (configured as read-only) was added via the 'Local Network' option in the VLC app.
The NFS share's directory and contents are displayed in the VLC app; however, when a video is selected, a "Playback error" results. Unfortunately, the error message is displayed for a fraction of a second, and is therefore illegible.
The NFS share is accessed via multiple computers, which employ the desktop version of VLC to play videos, so the share is functioning correctly. When copies of the videos are in local storage, they play without issue.
Why are the videos unplayable?
UPDATE: Audio files contained in the NFS share are able to be played without issue.