A small amount of the 3-(hexyldimethylammonio)propane-1-sulfonate zwitterionic side chain was integrated into a diketopyrrolopyrrole ambipolar polymer to modulate its field-effect carrier-transport characteristics. It was found that such a modification can strengthen the interchain interaction, promote crystallization, and thus improve the hole and electron mobilities by 3.9- and 8.2-fold, respectively.