Like wringing out a sponge, a metal-organic framework loaded with structure-changing light-responsive groups can squeeze out captured CO 2. Because of the groups being structurally integral, there is oscillation between native and excited states. Pairing with CO2 capture from coal-based power generation could reduce the parasitic energy load of adsorbent regeneration. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.