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I believe the problem stems from this issue in my event viewer:

Log Name:      Application
Source:        Microsoft-Windows-User Profiles Service
Date:          5/30/2015 3:19:04 PM
Event ID:      1501
Task Category: None
Level:         Error
Keywords:      
User:          Daniel-PC\daniel2
Computer:      Daniel-PC
Description:
Windows cannot create a temporary profile directory. This problem may be caused by insufficient security rights. 

 DETAIL - The system cannot find the path specified.

When my computer starts up, and logs in for the first time, (I believe) it's trying to create a backup for this profile. This fails, and then I get the dreaded "User Profile Service Failed". I can then login to a different account, check the registry, and restore the .bak registry entry in HKEY_LOCAL_MACHINE\SOFTWARE\Microsoft\Windows NT\CurrentVersion\ProfileList\, and then I'm able to login. After a restart (Not a logoff suprisingly), this issue occurs again.

Some things to note about this Windows install: I modified the users profile directory and the ProgramData directories from the C: drive to my external USB drive following the steps here.

Where I'd like to go from here: I'd like to debug the user profiles services some more (gpsvg.log appears to be of no help, and trying to enable diagnostic logs on the User Profile Service via Event Viewer showed no useful logs). I'd like to see where the copy is failing, and what directory it's trying to move to, to try and figure this out further.

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