Rigorously designed sub-micrometer structure arrays are widely used in metasurfaces for light modulation. One of the glaring restrictions is the unavailability of easily accessible fabrication methods to efficiently produce large-area and freely designed structure arrays with nanoscale resolution. We develop a patterned pulse laser lithography (PPLL) approach to create structure arrays with sub-wavelength feature resolution and periods from less than 1 μm to over 15 μm on large-area thin films with substrates under ambient conditions. Separated ultrafast laser pulses with patterned wavefront by quasi-binary phase masks rapidly create periodic ablated/modified structures by high-speed scanning. The gradient intensity boundary and circular polarization of the wavefront weaken diffraction and polarization-dependent asymmetricity effects during light propagation for high uniformity. Structural units of metasurfaces are obtained on metal and inorganic photoresist films, such as antennas, catenaries, and nanogratings. We demonstrate a large-area metasurface (10 × 10 mm²) revealing excellent infrared absorption (3–7 μm), which comprises 250,000 concentric rings and takes only 5 minutes to produce.