My goal is to be able to move the mouse from the game to any other place on my desktop without having to click any buttons (alt+tab). Is this possible? I know of virtual PC there is a button that you can check that will lock/unlock the mouse.

You still have to Alt Tab to move off the Window.

And, you have to have another Window (any program or even Windows Explorer will do) in order to have something to Alt Tab too.

BTW, these games do not like to be Alt Tabbed, so always Save before you do this as it can lock up. It's not guranteed to lock up, but if you don't save first, you'll be crying in your Nuka Cola when it happens.

Another BTW, there is a mod that removes the window borders if you prefer to play this way. Windowed mode can be more stable and give higher FPS rates for some people.

When you say there is a mod to remove the border what are you referring too? Is this the ability to move the mouse freely ? Or just to remove the borders so all that shows is the game ?