I haven't used this so I cannot help.
Presuming that the returned TagLib.Tag can be cast to TagLib.Id3v2.Tag, the error that you are receiving could be solved with:
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TagLib.Id3v2.Tag tag = file.GetTag (TagLib.TagTypes.Id3v2) as TagLib.Id3v2.Tag;
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Try to get any image data to see what the returned format is, then you will decide how to display it. If it is a Bitmap object, then you can pass it to
PictureBox.Image property and you're done. If not, then you will have to find or implement some conversions.