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Four efficient artificial light-harvesting systems have been developed in the present work. They assemble sodium dodecyl sulphate (SDS) with organic small molecule chromophores to synthesize microcrystals to mimic chlorophyll. In microcrystals, the chromophores are ordered through intermolecular dipole-dipole interactions, which results in efficient energy transfer. In the D-2/A-2 light-harvesting system, the donor concentrates excitation energy from 500 chromophores into a single acceptor with a relative high energy transfer efficiency (86%) and an antenna efficiency (33). The microcrystals exhibit high energy harvesting performance and act as an ideal framework for artificial light-harvesting systems. We have developed four light-harvesting systems (LHSs) using microcrystals composed of organic small molecule chromophores to mimic chlorophyll. In microcrystals, the chromophores are ordered through intermolecular dipole-dipole interactions, which results in efficient energy transfer. [Display omitted] • Four efficient LHSs have been developed using nanocrystals composed of organic chromophores to simulate chlorophyll. • The nanocrystals were co-assembled with the donor and accepter at a controlled ratio with rod-like structures. • In the nanocrystals, the chromophores were highly ordered through dipole-dipole interactions between molecules. • The LHS showed a high energy transfer efficiency (89%) and a high antenna efficiency (33). [ABSTRACT FROM AUTHOR]