In this work, we present a comprehensive theoretical and experimental study of quantum confinement in layered platinum diselenide (PtSe 2 ) films as a function of film thickness. Our electrical measurements, in combination with density functional theory calculations, show distinct layer-dependent semimetal-to-semiconductor evolution in PtSe 2 films, and highlight the importance of including van der Waals interactions, Green's function calibration, and screened Coulomb interactions in the determination of the thickness-dependent PtSe 2 energy gap. Large-area PtSe 2 films of varying thickness (2.5-6.5 nm) were formed at 400°C by thermally assisted conversion of ultra-thin platinum films on Si/SiO 2 substrates. The PtSe 2 films exhibit p-type semiconducting behavior with hole mobility values up to 13 cm 2 /V·s. Metal-oxide-semiconductor field-effect transistors have been fabricated using the grown PtSe 2 films and a gate field-controlled switching performance with an I ON /I OFF ratio of >230 has been measured at room temperature for a 2.5-3 nm PtSe 2 film, while the ratio drops to <2 for 5-6.5 nm-thick PtSe 2 films, consistent with a semiconductingto-semimetallic transition with increasing PtSe 2 film thickness. These experimental observations indicate that the low-temperature growth of semimetallic or semiconducting PtSe 2 could be integrated into the back-end-of-line of a silicon complementary metaloxide-semiconductor process.npj 2D Materials and Applications (2019) 3:33 ; https://doi.