Carbon neutrality is increasingly broadly recognized as a vehicle for climate action and sustainable development. Photosynthesis contributes to maintaining a suitable carbon-oxygen balance for survival and plays an irreplaceable role in mitigating the greenhouse effect. However, the energy conversion efficiency of photosynthesis is only about 1%, far below the theoretical maximum. With the ecological demand of carbon neutrality, it is wise and necessary to further improve the efficiency of photosynthesis. Among methods to do so, the most direct and original one is improving the utilization of photosynthetic pigments to the weak absorption region of the spectrum and thus enhancing the solar energy utilization efficiency.This Account summarizes our group's work on constructing conjugated polymer-photosynthetic organism interfaces to augment photosynthetic efficiency. Side chain modification of ionic groups or preparation of nanoparticles makes conjugated polymers water-soluble and electrically charged, which allows them to bind to the surface of photosynthetic microorganisms through electrostatic interactions or be absorbed by plant roots. Owing to the designable and unparalleled light capture and emission capabilities, funnel-like excitation energy transfer mode, and enviable biocompatibility, organic semiconductor conjugated polymers can be used as "artificial antennas" to make up for the lack of natural antenna pigments and expand the photosynthetically active radiation (PAR) range. With this strategy, we achieved enhancement of the photosynthetic efficiency of a broad range of organisms, including oxygenic photosynthetic organisms, from organelle to prokaryotic cyanobacteria, eukaryotic lower plants, and higher plants, as well as anoxygenic photosynthetic organisms. Unlike conventional semiconductors, conjugated polymers have not only electronic conductivity but also ionic conductivity, which is the main means of bioelectrical signal transduction. Therefore, they are able to act as "electron bridges" to accelerate the electron transfer rate at the material-organism interface. On this basis, we introduced conjugated polymers into artificial photosynthesis systems, including biological photovoltaics and artificial carbon sequestration, to increase energy conversion efficiency. These studies open a new frontier for functional studies of conjugated molecules and provide inspirations for the design of photosynthesis systems in the future.