iCloud Drive stupidly fills your whole local Mac disc. And no documentation by Apple how it works. Dropbox, Google Drive and OneDrive the same stupid behaviour and lack of documentation what happens if the data in the cloud is bigger than your local disc. Dropbox SmartSync is only for business teams. Google Stream Drive the same and additional only for early adopters with invitation. OneDrive had the feature only back with Windows 8.
On mobile devices all the services let you access all your data; as it should.
With macOS 10.12 Sierra (September 2016) you can enable Smart Sync for the folders Desktop and Documents. The bad thing about the documents folder it is trashed by app data (1,5 Gbyte Microsoft user data, mountains of Gbyte VirtualBox VMs) I don't want in my iCloud Drive. That's why I never used the Documents folder for my important files.
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If you don't want screenshots created on the desktop, but in the folder Downloads (or elsewhere) execute the following in the Terminal:
defaults write com.apple.screencapture location ~/Downloads/
Add your Desktop and Documents files to iCloud Drive
How iCloud Drive Should Work, But Doesn’t
On mobile devices all the services let you access all your data; as it should.
With macOS 10.12 Sierra (September 2016) you can enable Smart Sync for the folders Desktop and Documents. The bad thing about the documents folder it is trashed by app data (1,5 Gbyte Microsoft user data, mountains of Gbyte VirtualBox VMs) I don't want in my iCloud Drive. That's why I never used the Documents folder for my important files.
defaults write com.apple.screencapture location ~/Downloads/
Add your Desktop and Documents files to iCloud Drive
How iCloud Drive Should Work, But Doesn’t