Generally, yes. Move the documents in the One Drive folder that you do not want sync'd to another, different folder. Leave the documents you do want sync'd in the One Drive folder.

Move other folders you do want sync'c into the One Drive main folder.

It may help your thinking to give One Drive folder different names so you can distinguish.

I have different folder in my One Drive "Library" than in my Documents "Library" .

I use both Drop Box and One Drive and the ideas above service me well.

Generally, yes. Move the documents in the One Drive folder that you do not want sync'd to another, different folder. Leave the documents you do want sync'd in the One Drive folder.

Move other folders you do want sync'c into the One Drive main folder.

It may help your thinking to give One Drive folder different names so you can distinguish.

I have different folders in my One Drive "Library" than in my Documents "Library" .

I use both Drop Box and One Drive and the ideas above service me well.