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OneDrive - How to Sync a Folder outside OneDrive folders
By default, OneDrive syncs folders that are under its folder in Windows. If you want to sync a folder which is outside the OneDrive folder, you have to move it under OneDrive folder. There is a workaround to achieve this, keep reading...
In this example, below are the folders
The OneDrive sync folders are in:
C:\Users\Username\OneDrive
The folder you want to sync is outside above path, it's:
C:\Files
Follow the below steps...
Open an Admin command prompt by Clicking on Windows Start button and Click Command Prompt (Admin)

2. Navigate to the folder where you want to create a Symbolic link (Source), in this case, C:\Users\Username\OneDrive
3. Run the below command in the below screenshot, A symbolic link is created to C:\Files folder

4. I created a Test.txt file in SampleLinkFolder folder (under C:\Users\OneDrive) and the same file can be seen in C:\Files in below screenshot

How to Remove the Symbolic Link / Stop backing up C:\Files folder in OneDrive?
If you want to remove the symbolic link, run the below command
rd SampleLinkFolder