Nanocrystals have exhibited unique optoelectronic properties and demonstrated a wide range of applications in light-emitting devices, semiconductor devices and solar cell devices. However, previous studies usually deposit nanocrystal films on traditional rigid substrates, limiting their applications in large-scale, direct-deposited flexible device fabrication processes, such as roll-to-roll printing process. Here, we report a direct deposition method for lead sulfide (PbS) nanocrystal films on flexible polymer substrates. By adding triethanolamine-coordinated Pb precursors to the reaction system to enhance the adhesion to the substrate and controlling the precursor ratios, we obtained high-quality flexible PbS films. The film is composed of octahedral PbS nanocrystals with preferred (111) orientation. The optical band gap of the nanocrystal films can be tuned from 1.32 eV to 1.60 eV by adjusting the ratio of the precursors, and an ideal band gap of 1.4 eV for single-junction solar cells was also obtained when Pb to S ratio reaches 1.4:1. More importantly, the flexible PbS films exhibit high charge carrier mobility of up to 25 cm2 V[Formula: see text] s[Formula: see text], which is comparable to that of PbS films grown on traditional rigid substrates (e.g. silicon wafers or glasses). To our knowledge, this mobility is also the highest for PbS fabricated directly on flexible substrates. Our study provides a new approach for the preparation of low-cost and roll-to-roll processable nanocrystal films for future flexible optoelectronic devices.