We report the use of thiocyanate as a ligand for lead sulfide (PbS) nanocubes for high-performance, thin-film electronics. PbS nanocubes, self-assembled into thin films and capped with the thiocyanate, exhibit ambipolar characteristics in field-effect transistors. The nearly balanced, high mobilities for electrons and holes enable the fabrication of CMOS-like inverters with promising gains of ∼22 from a single semiconductor material. The mild chemical treatment and low-temperature processing conditions are compatible with plastic substrates, allowing the realization of flexible, nonsintered quantum dot circuits.