Herein, we report a novel method for constructing polymeric conjugated radicals, introducing an open-shell benzobisthiadiazole (BBT) unit to a (3E,7E)-3,7-bis(2-oxo-1H-pyrrolo-[2,3-b]pyridine-3(2H)ylidene)benzo[1,2-b:4,5-b′]difuran-2,6-(3H,7H)-dione-alt-(E)-1,2-di(thiophen-2-yl)ethene polymeric conjugated backbone (P1 with closed-shell structure) affording conjugated polymers P2−P4 with open-shell characteristics.Through this method, the spin characteristic of the polymer conjugated radicals can also be easily tuned, in which the spin concentration of P2−P4 increases with the increase of the BBT ratio. Moreover, P2−P4 have narrowed energy gaps and n-type charge transport properties with electron mobilities of 0.12−0.35 cm 2 V −1 s −1 , comparable to or higher than those of BBT-containing conjugated polymers reported so far. Microstructural investigations indicated that the gradual decrease of μ e from P1 to P4 originates from their BBT-caused deteriorating molecular aggregations in solid thin films. Our results show that incorporating an open-shell moiety into a high-performance conjugated backbone is a promising method for developing polymeric conjugated radicals with high mobility and tunable open-shell character.