Wow. That's a lot of files! It is very suspicious that it is the NetworkService's user profile that is filling up with Temporary Internet Files, and not your user profile. This suggests that some service was accessing the Internet via Internet Explorer
or an Internet Explorer ActiveX control. Incidentally, my computer's NetworkService Temporary Internet Files folder is completely empty.
For now, I am going to assume that any infection has been removed, and we just need to clean out its payload. I wrote a program that is specifically designed to delete massive amounts of files, and files where the pathnames are too long, both which
are scenarios that Explorer does not handle too well. If you have not already been successful clearing out that folder, please:
- Cancel any delete operations currently in progress.
- Download my program: DeleteFolderTree.exe (42 KB standalone portable application).
- Copy the path to the errant folder: C:\Windows\ServiceProfiles\NetworkService\AppData\Local\Microsoft\Windows\Temporary Internet Files\Content.IE5
- Paste it into my program and click [Delete].
Unlike Explorer, my program won't have a "Preparing to delete" period; it will start deleting files/folders immediately after confirmation from you. Unfortunately, there will also be no progress indication, only a count of deleted/failed items, and
a readout of the increasing amount of free disk space. This is due to my program's skipping file enumeration, which is what took TreeSize so long, and is what Explorer is doing during the "Preparing to delete" phase. My program does the enumeration and deletion
at the same time, which means it never knows how many files are left to delete.

@Frederik Long and
HairyFool: I know you guys were trying to be helpful, but if a user changes the Temporary Internet Files cache size setting, if will only affect
their user profile. In this case, since it is the NetworkService profiles' Temporary Internet Files cache that is getting out of hand, changing that setting won't help at all.