A second file can be found in the Fallout4 subfolder called Fallout4Prefs.ini. Not only do you have to disable VSync in the driver, you will have to change iPresentInterval=1 to iPresentInterval=0 in the Fallout4_Default.ini file found in the Fallout 4 game folder (located in the Steamapps/common folder). For reasons unknown to us, the AMD Catalyst driver doesn't override the game, despite having essentially the same function within the driver suite. To disable VSync on systems powered by AMD graphics cards, the process involves editing a single parameter found in multiple. This was all that was necessary for Nvidia GPUs, but it wasn't so simple for AMD GPUs. By default, the driver lets the application control this setting, but you can override it to disable VSync. Within those settings, found in the Manage 3D Settings section of the Nvidia Control Panel, there is an option to disable Vertical Sync.
The GeForce drivers allow for specific graphics settings for individual games.
With the systems running Nvidia cards, this proved to be extremely simple.