What makes an FLP a good catalyst? Thus far, a number of frustrated Lewis pairs (FLPs) are reported in the literature, but not all of them activate molecular hydrogen. This phenomenon has been addressed by the physical-organic investigation of the Lewis base as component in an FLP catalyst. The FLP′s performance in the autoinduced hydrogenation is intrinsically dependent on the electron-donating ability of the Lewis base providing a detailed structure–reactivity relationship in FLP catalysis. More information can be found in the Full Paper by J. Paradies et al. on page 7422 ff.