Photosystem II (PSII) is a photoactive protein that can drive water oxidation under light irradiation. Recently, PSII has been broadly investigated with the high demand on the bioenergy. Here, we demonstrate a facile approach for the fabrication of a photoactive electrode by the integration of PSII with quantum dots (QDs)/polyelectrolyte multilayers. The assembled QDs and PSII film with a polyelectrolyte based substrate via layer-by-layer assembly can remain the photoactivity of the PSII and broaden the absorption spectrum of PSII to produce a high photocurrent yield. The co-assembly exhibits an obviously enhanced photocurrent under UV light irradiation. The proposed strategy can be considered for the reference and usage of PSII toward the solar energy conversion.