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The iMac is Thunderbolt and my MBP is not, so I can't use Target Display Mode, but I'd like to use the bigger screen. Can I make my MBP a larger-than-native resolution?
Better yet, can I share a second, virtual screen at the iMac's resolution and use the built-in screen at its native resolution as a side monitor?
I doubt you could set the primary display to bigger than that of your iMac, however I know some programs (Off the top of my head 'air display') create a virtual second display. Air Display is an iOS app however...I'm not sure it would be able to handle a 2560x1440 resolution.
Something you could try is remote connecting to your MacBook Pro from your iMac. This could possibly allow you to make it a large resolution.
