A newly introduced two-dimensional (2D) layered germanium arsenide (GeAs) has attracted growing interest due to its promising highly in-plane anisotropic crystal structure and electronic properties for photonic and optoelectronic applications. The potential of 2D layered GeAs for many applications such as anisotropic photodetection, electronics, superconductivity and thermoelectricity is being investigated in recent studies. However, the intrinsic nonlinear optical properties of 2D layered GeAs have not been explored yet. Here, thickness-and incident polarization-dependent in-plane anisotropic third-harmonic generation (THG) from the mechanically exfoliated thin GeAs flakes is reported. Furthermore, the effect of the flake thickness on the THG conversion efficiency is shown to find the optimal thickness range for high conversion efficiency. The polarization state of the emitted THG signal is also analyzed by measuring the Stokes parameters with different polarization states of the pump beam to demonstrate the capability of controlling the intensity and polarization of TH emission. our results will create new opportunities for advancing anisotropic optical devices used for future photonic integration, optical communication and optical information processing. Nonlinear optical materials play a progressively significant role on the development of important photonic devices, for example, ultrafast lasers 1 , soliton generators 2 , optical modulators 3 and optical multiplexers 4 , which are extensively used in many applications of medicine, industry, communication and imaging 4,5. Although the traditional bulk nonlinear optical materials such as beta barium borate (β-BaB 2 O 4) 6 and lithium niobite (LiNbO 3) 3 have been widely used, these materials are greatly limited by low conversion efficiency, low nonlinear optical susceptibility and bulky crystal size. It is crucially important to search for nonlinear optical materials with both high conversion efficiency and compact crystal size, which can be integrated into the future nanoscale photonic and quantum chips 7-9. Within this scope, 2D materials have been the most promising candidates to fulfill these demands 10. The emerging 2D layered materials are currently at the center of intensive research efforts owing to their superior physical properties such as high carrier mobility 11,12 , broadband optical response 13 , large Young's modulus 14,15 and high thermal conductivity 16. In addition, the broad optical spectral range covered by 2D materials make them very promising for photonic and optoelectronic applications 17. Besides the linear optical properties, 2D materials exhibit strong optical nonlinearities which endows them as promising nonlinear optical materials 10,18,19 which have been used for saturable absorption (SA) 20 , second-harmonic generation (SHG) 21 , THG 22,23 , self-phase modulation 24,25 , nonlinear Kerr effect 26,27 and four-wave mixing (FWM) 28. Beyond graphene, 2D transition metal dichalcogenides (TMDs) such as MoS 2 21,29-31 and WSe 2 32,33 , he...