We present a smart strategy to simultaneously increase the short circuit current (J sc ), the open circuit voltage (V oc ), and the fill factor (FF) of polymer solar cells (PSCs). A twodimensional conjugated small molecule photovoltaic material (SMPV1), as the second electron donor, was doped into the blend system of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C71butyric acid methyl (PC 71 BM) to form ternary PSCs. The ternary PSCs with 5 wt % SMPV1 doping ratio in donors achieve 4.06% champion power conversion efficiency (PCE), corresponding to about 21.2% enhancement compared with the 3.35% PCE of P3HT:PC 71 BM-based PSCs. The underlying mechanism on performance improvement of ternary PSCs can be summarized as (i) harvesting more photons in the longer wavelength region to increase J sc ; (ii) obtaining the lower mixed highest occupied molecular orbital (HOMO) energy level by incorporating SMPV1 to increase V oc ; (iii) forming the better charge carrier transport channels through the cascade energy level structure and optimizing phase separation of donor/acceptor materials to increase J sc and FF.