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The nonlinear refractive index of the rectangular layered MoS2 and the nano-MoS2/TiO2 composite was performed by the spatial self-phase modulation (SSPM) and the Z-scan,respectively.In the SSPM experiments,the nonlinear refractive index of rectangular layered MoS2 dispersion was acquired to be 3.17× 10-5 cm2/W,which is larger than that of the nano-MoS2/TiO2 composite dispersion 2.66×10-5 cm2/W and that of the arbitrarily shaped MoS2 dispersion 2.88×10-6 cm2/W.The principal mechanism is that the laser-induced wind-chime shaped reorientation of nanoflakes results in the emergence of the nonlocal electron coherence,which enhances the nonlinear optical properties of the 2D nanoflakes dispersion.For Z-scan measurements,the nonlinear refractive index of the nano-MoS2/TiO2 composite thin film 3.6× 10-9 cm2/W is larger that of the rectangular layered MoS2 thin film 2.6× 10-9 cm2/W.The enhanced principal mechanism is that wide bandgap TiO2 nanoparticles modulated the band structure of the narrow bandgap MoS2,thus enhances its nonlinear optical properties.This research confirms the possibility of the existence of wind-chime shaped alignment in SSPM and provides two different paths for the enhancement of the nonlinear optical properties of MoS2.