One way would be assign a category value to the files in these two folders. In Mezzmo, click on one of the folders you mention to display all the files. Select all the files (using Ctrl or Shift + click, or using Ctrl+A) and right-click on one of the selected files and click Properties. On the Properties dialog, enter a value into the 'Category' edit box such as "watching". Click OK. This will save that category value into all selected files. Repeat the steps for the other folder's files. Now edit your smart playlist. Set the rule to be:
Match [all] rules:
[Category][contains][watching]
[Play Count][is not][0]
This will list all files with that category that have not yet been played .
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