Infrared gradient refractive index (GRIN) lenses have great application value and potential in multispectral imaging systems. This study reports various chalcogenide axial GRIN glasses prepared using the hot‐pressing diffusion method. It is worth noting that the S4–S60 GRIN sample has a difference in refractive index (RI) Δn of greater than 0.3 and a diffusion depth of about 5 mm, which is the deepest diffusion depth reported in chalcogenide glass to date. In addition, the linear portion in the profile of the GRIN sample has a RI difference of 0.15 and a thickness of 1.2 mm. The effects of the temperature, concentration difference, and diffusion time on the sample diffusion process are discussed. The dispersion properties of the GRIN samples were further calculated, providing a new option for correcting chromatic aberrations in optical systems. In addition, a method for the indirect nondestructive characterization of sample RI using the Raman intensity ratio is proposed, and the reliability of the method is verified by practical experiments, which is convenient for the subsequent measurement of the GRIN profile.