In this paper, 4-(dicyanomethylene)-2-t-butyl-6(1,1,7,7-tetramethyljulolidyl-9-enyl)-4H-pyran (DCJTB) has been used in interface modification of dye-sensitized solar cells (DSCs) with combined effects of retarding charge recombination and Förster resonant energy transfer (FRET). DCJTB interface modification significantly improved photovoltaic performance of DSCs. I–V curves shows the conversion efficiency increases from 4.27% to 5.64% with DCJTB coating. The application of DCJTB with combined effects is beneficial to explore more novel multi-functional interface modification materials to improve the performance of DSCs.