unfortunately you can't do what you want to do. Damn it would be nice, I'd have all my games here.
I know your annoyance. I have 80+ game and 5 kids and a wife that all game.
The funny thing is upto 5 years ago you could have been able to play 2 different games on two different computers.
Your Options are to use your account in offline mode
or
Rebuy the games
or
Use an Emulator to run the Steam Games sans Steam.
And I will hunt down and skin alive (Well vigorously ex-foliate) anyone that suggests using Steam Family Sharing. Then use their hide (well dried skin flakes) to make a person shaped banner that explains SFS does not let simultaneous use of different games.
PookaMustard: I don't know of any game that allows you to move from Steam to GOG... I'd appreciate this function, but....
MAy be these?
http://www.gog.com/reclaim oh and Witcher 1 and 2.
Some games with Keys can be activated on Origin, I did that with bullet storm and some others.
And Origin will let you play different (or even some of the same) games at the same time. Score 1 for the most evil company in the world.