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The highly promising linear and nonlinear optical properties of innovative thin films of GeSe1–xTex chalcogenide materials in the amorphous as‐deposited state, and after crystallization, are revealed here. These innovative alloys bridge the gap between two families of materials: chalcogenide glasses (GeSe) and phase‐change materials (GeTe). Their unique optical properties make them attractive candidates for reconfigurable and nonlinear photonic applications in the infrared. In this context, it is shown how, by varying the Te content of GeSe1–xTex thin films, it is possible to tailor their linear and nonlinear optical properties to optimize them for a wide range of innovative applications. [ABSTRACT FROM AUTHOR]