The Cover Feature shows the transformation of a bis‐phosphonium ylide molecule to a medium‐sized cyclic olefin under visible‐light activation. The photoredox activation of ylides features an umpolung reactivity of the classical nucleophile in coupling reactions with other ylide partners. Successful one‐pot olefination from activated halides is also demonstrated in the article. More information can be found in the Communication by Xue‐Wei Liu et al. on page 93 in Issue 1, 2019 (DOI: 10.1002/ajoc.201800586).