AbstractOptical metasurfaces, consisting of subwavelength‐scale meta‐atom arrays, hold great promise of overcoming the fundamental limitations of conventional optics. Due to their structural complexity, metasurfaces usually require high‐resolution yet slow and expensive fabrication processes. Here, using a metasurface polarimetric imaging device as an example, the photonic structures and the Nanoimprint lithography (NIL) processes are designed, creating two separate NIL molds over a patterning area of > 20 mm2 with designed Moiré alignment markers by electron‐beam writing, and further subsequently integrate silicon and aluminum metasurface structures on a chip. Uniquely, the silicon and aluminum metasurfaces are fabricated by using the nanolithography and 3D pattern‐transfer capabilities of NIL, respectively, achieving nanometer‐scale linewidth uniformity, sub‐200 nm translational overlay accuracy, and <0.017 rotational alignment error while significantly reducing fabrication complexity and surface roughness. The micro‐sized multilayer metasurfaces have high circular polarization extinction ratios as large as ≈20 and ≈80 in blue and red wavelengths. Further, the metasurface chip‐integrated CMOS imager demonstrates high accuracy in broad‐band, full Stokes parameter analysis in the visible wavelength ranges and single‐shot polarimetric imaging. This novel, NIL‐based, multilayered nanomanufacturing approach is applicable to the scalable production of large‐area functional structures for ultra‐compact optic, electronic, and quantum devices.