We demonstrate a versatile top-down ion exchange process, done at ambient temperature, to form epitaxial chalcogenide films and devices, with nanometer scale thickness control. To demonstrate the versatility of our process we have synthesized (1) epitaxial chalcogenide metallic and semiconducting films and (2) free-standing chalcogenide films and (3) completed in situ formation of atomically sharp heterojunctions by selective ion exchange. Epitaxial NiCo2S4 thin films prepared by our process show 115 times higher mobility than NiCo2S4 pellets (23 vs 0.2 cm(2) V-1 s(-1)) prepared by previous reports. By controlling the ion exchange process time, we made free-standing epitaxial films of NiCo2S4 and transferred them onto different substrates. We also demonstrate in situ formation of atomically sharp, lateral Schottky diodes based on NiCo2O4/NiCo2S4 heterojunction, using a single ion exchange step. Additionally, we show that our approach can be easily extended to other chalcogenide semiconductors. Specifically, we used our process to prepare Cu1.8S thin films with mobility that matches single crystal Cu1.8S (25 cm(2) V-1 s(-1)), which is ca. 28 times higher than the previously reported Cu1.8S thin film mobility (0.58 cm(2) V-1 s(-1)), thus demonstrating the universal nature of our process. This is the first report in which chalcogenide thin films retain the epitaxial nature of the precursor oxide films, an approach that will be useful in many applications.