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To solve the issue of the contradiction between photovoltaic power generation and plant photosynthesis for sunlight demand, we propose a design method of multi-passband polymer multilayer optical structure. Using polycarbonate (PC) and polymethyl methacrylate (PMMA), two polymer materials with different refractive indices, the passband position and passband bandwidth are calculated and adjusted by the transmission matrix method and TFCalc software. A 450 nm, 660 nm, and 730 nm three-passband filter was realized by superimposing stacks of different band positions. The feasibility of the photovoltaic agriculture was confirmed by the power generation efficiency and the actual plant growth.