•A two-photon absorption compound, DMDP-CH2Br, was synthesized and linked to LHC-II.•The LHC-II-dye complex can absorb two photons of the laser light effectively.•The absorbed energy in the LHC-II-dye complex can transfer to chlorophyll a.The plant light-harvesting complexes of photosystem II (LHC-II) play important roles in collecting solar energy and transferring the energy to the reaction centers of photosystems I and II. A two photon absorption compound, 4-(bromomethyl)-N-(4-(dimesitylboryl)phenyl)-N-phenylaniline (DMDP-CH2Br), was synthesized and covalently linked to the LHC-II in formation of a LHC-II-dye complex, which still maintained the biological activity of LHC-II system. Under irradiation with femtosecond laser pulses at 754 nm, the LHC-II-dye complex can absorb two photons of the laser light effectively compared with the wild type LHC-II. The absorbed excitation energy is then transferred to chlorophyll a with an obvious fluorescence enhancement. The results may be interesting and give potentials for developing hybrid photosystems.Graphical abstractA two photon absorption compound, 4-(bromomethyl)-N-(4-(dimesitylboryl)phenyl)-N-phenyl-aniline (DMDP-CH2Br), was synthesized and covalently linked to the LHC-II in formation of a LHC-II-dye complex. The LHC-II-dye complex can absorb two photons of the laser light effectively. The absorbed excitation energy is then transferred to chlorophyll a with an obvious fluorescence enhancement. The work may be interesting and give potentials for developing hybrid photosystems.