For your changes to be effective, you'll need to force Amahi to regenerate the greyhole.conf file. You can do so by editing a share, clicking it's path, and just clicking the Save button without actually changing the path.
== Copying you your data into Greyhole shares the first time ==
When you start using Greyhole, you might want to copy or move all your exiting files into your new shares that use the storage pool.