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An artificial light‐harvesting system with sequential energy‐transfer process was fabricated based on a supramolecular strategy. Self‐assembled from the host–guest complex formed by water‐soluble pillar[5]arene (WP5), a bola‐type tetraphenylethylene‐functionalized dialkyl ammonium derivative (TPEDA), and two fluorescent dyes, Eosin Y (ESY) and Nile Red (NiR), the supramolecular vesicles achieve efficient energy transfer from the AIE guest TPEDA to ESY. ESY can function as a relay to further transfer the energy to the second acceptor NiR and realize a two‐step sequential energy‐transfer process with good efficiency. By tuning the donor/acceptor ratio, bright white light emission can be successfully achieved with a CIE coordinate of (0.33, 0.33). To better mimic natural photosynthesis and make full use of the harvested energy, the WP5⊃TPEDA‐ESY‐NiR system can be utilized as a nanoreactor: photocatalyzed dehalogenation of α‐bromoacetophenone was realized with 96 % yield in aqueous medium. [ABSTRACT FROM AUTHOR]