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My current installation of Windows 10 already has the Users directory on another hard disk.

When I installed Windows in this computer, I used the sysprep method to move the Users directory to the D: drive.

Now I need to move the contents of the D: drive to a bigger hard disk, but when I tried to robocopy its contents to a new hard disk and assign it the D: letter I could not sign in to any of the existing accounts.

What steps am I missing here?

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There are handful of odd structures within user profile directories like junctions and symlinks, and robocopy needs to be instructed how to handle them. You can try the example command from the answer here - specifically, include the /SJ and /SL flags:

robocopy D:\Users E:\Users /E /COPYALL /SJ /SL /DCOPY:DATE /R:3 /W:5

Another option you can try is simply cloning the entire D: disk over to the new drive using a tool like Clonezilla.

Note that moving the Users directory to another location like this is not recommended or supported by Microsoft, even when using sysprep

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