Two-dimensional organic materials are mainly constructed by using orthogonal anisotropic connectivity of covalent bonding and π-π stacking. The noncovalent connectivity between building blocks is presumed to be too delicate to stabilize the two-dimensional (2D) layers. Contrary to this assumption, we constructed graphite-like 2D layered material by utilizing pure noncovalent connectivity, i.e., weak intermolecular and π-π interaction via a molecular Tetris strategy. We produce X-ray mountable single crystals comprising polycyclic aromatic heterocycles by employing a single-crystal-to-dissolution-to-single-crystal transformation methodology. The macromechanical analysis of this layered crystal shows shearing behavior, which is quantified using nanoindentation experiments. The 2D lattice’s layer space allows reversible intercalation-deintercalation of iodine, which enhances the photoconductivity by 17 folds. Combined efforts of X-ray diffraction, solid-state spectroscopy, and electrochemical studies established the mechanism of intercalation and resulting photoconductivity enhancement.