2D anisotropic materials, typically consisting of 1D distorted chains arranged in parallel or anti-parallel patterns, are gaining attention for their potential in anisotropic electronic and optoelectronic devices. 2D anisotropic materials with cross-stacked interconnected 1D chains will show improved anisotropy and stability. Nonetheless, to date, no 2D anisotropic materials featuring cross-stacked motifs have been experimentally realized. This work identifies AgTiPS