Carbon nanotubes/graphene with specific nitrogen doping can contribute to a controllable, highly selective, and reversible CO2 capture, as illustrated by the front cover image. Carbon recycling represents a fundamental aspect of the global carbon balance, with CO2 capturing the first key concept of this cycle. Prof. Zhonghua Zhu and co-workers use long range dispersion-corrected density functional theory calculations to reveal that pyridinic nitrogen on carbon nanotubes/graphene leads to an increased CO2 adsorption strength in the presence of injected electrons, and, hence, a highly selective adsorption of CO2 over N2. This functionality can induce intrinsically reversible CO2 adsorption by switching the charge carrying state of the system on/off. More detail is given in the Full Paper by Jiao et al. on page 435, while more information about the research group is available in the Cover Profile (DOI: 10.1002/cssc.201301349).