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We studied the third-order nonlinear (TONL at 0.8 μm) properties of the chalcogenide glass-ceramic within the GeS2-Sb2S3–CsCl system, and found that the nano-crystallization of CsCl phase in the glass matrix could enhance the TONL properties significantly. As compared to the parent glass without crystallization, the maximum nonlinear refractive index (n2) of the GeS2-Sb2S3–CsCl chalcogenide glass ceramics is nearly tripled, while the maximum nonlinear absorption coefficient (β) is also increased by 62%. The calculation of figure of merits (FOMs) ascertained that glass ceramics embedded with smaller CsCl crystallites tend to have better TONL performance.