The search for semiconductors that can be solution-processed into thin-film form at low temperature, while simultaneously providing quality device characteristics, represents a significant challenge for materials chemists. Continuous thin films with field-effect mobilities of 10 cm2 V−1 s−1 or greater are particularly desirable for high-speed microelectronic applications. Attainment of this goal should provide important opportunities for electronic devices, including potentially low-cost, large-area and flexible computing devices, displays, sensors and solar cells. While the majority of work toward this goal has focused on organic semiconductors (both molecular and polymeric), with highest reported mobilties in the range of 1 cm2 V−1 s−1, this review will address recent developments in the search for semiconductors with extended inorganic frameworks (offering the potential for higher mobility) that can be processed from solution using high-throughput, low-cost and low-temperature techniques such as spin-coating, printing or stamping. Two areas of recent interest will be highlighted – tin(II) iodide based organic–inorganic hybrids and soluble chalcogenide semiconductors. Application of the resulting thin films in devices will primarily be discussed in terms of thin-film field-effect transistors (TFTs), although other device applications can be envisioned.