Two novel-aqueous artificial light-harvesting platforms (ALHPs) with high efficiency have been successfully developed based on supramolecular interactions with salicylideneaniline derivative (PPA), water-soluble-pillar [5]arene (WP5), Phloxine B (PHB), and sulforhodamine 101 (SR101). After PHB and SR101 loaded in WP5⊃PPA nanoparticles, the constructed WP5⊃PPA-PHB and WP5⊃PPA-SR101 ALHPs exhibited excellent quantum yields (ΦQY) and antenna effects (AE), which were 24.19% and 33.6 for WP5⊃PPA-PHB, 31.23% and 38.7 for WP5⊃PPA-SR101. Significantly, cell cytotoxicity experiments displayed that WP5⊃PPA-SR101 nanoparticles were biocompatible with NIH 3T3 normal cells. Moreover, CLSM results further confirmed their co-location imaging abilities of PPA and SR101 because of FRET process, exhibiting potential prospects in bio-imaging materials.