Yes, you could use the plugin to resolve the old site URLs to the new location on your WordPress site. The one thing to remember is that the old domain name has to be the same as the new one (i.e., the old one would be http://something.com/oldpage.htm and the new one would be http://something.com/newpage/ - as you can see the domain is the same - using a different domain will not work).
You can import a list of redirects. You can set them up in Excel, but you need to export them as a Pipe delineated text file before you upload in this layout, one per line:
For example, the upload file would be something like:
and you would use the "Add to Quick Redirect Option" to upload.