Constructing nanoparticles into well-defined structures at mesoscale and larger to create novel functional materials remains a challenge. Inspired by atomic epitaxial growth, we propose an epitaxial assembly method to form two-dimensional nanoparticle arrays (2D NAs) directly onto desired materials. As an illustration, we employ a series of surfactant-capped nanoparticles as the artificial atoms and layered hybrid perovskite (LHP) materials as the substrates and obtain 2D NAs in a large area with few defects. This method is universal for nanoparticles with different shapes, sizes, and compositions and for LHP substrates with different metallic cores. Raman spectroscopic and X-ray diffraction data support our hypothesis of epitaxial assembly. The novel method offers new insights into the controllable assembly of complex functional materials and may push the development of materials science at the mesoscale.