In order to sync a file/folder from your computer to the cloud, you have to move that file/folder into the "Creative Cloud Files" folder. That is, you have to move them from their original place on your computer.

I propose to have a way to sync files directly from their original location in the computer. For some reference, this is what Google Drive does for example; as an addition to moving files into the folder, Google Drive gives you the option to sync files without moving them. They get uploaded into Google Drive and then you can sync them if you make any changes, which then get directly updated.