Colloidal InP quantum dots (QDs) have emerged as potential candidates for constructing nontoxic QD-based optoelectronic devices. However, charge transport in InP QD thin-film assemblies has been limitedly explored. Herein, we report the synthesis of ∼8 nm edge length (∼6.5 nm in height), tetrahedral InP QDs and study charge transport in thin films using the platform of the field-effect transistor (FET). We design a hybrid ligand-exchange strategy that combines solution-based exchange with S^2– and solid-state exchange with N₃^– to enhance interdot coupling and control the n-doping of InP QD films. Further modifying the QD surface with thin, thermally evaporated Se overlayers yields FETs with an average electron mobility of 0.45 cm² V^–1 s^–1, ∼10 times that of previously reported devices, and a higher on–off current ratio of 10³–10⁴. Analytical measurements suggest lower trap-state densities and longer carrier lifetimes in the Se-modified InP QD films, giving rise to a four-time longer carrier diffusion length.