Abstract: The challenges of nanotechnology are clear: reducing material requirements, significantly increasing efficiency, and improving stability. Through tailored nano-engineering, colloidal metasurfaces with template-assisted self-assembly can solve this challenge. Pre-synthesized nanoparticles, responsive polymers, and tailored templates form the backbone to produce functional metasurfaces on a large scale. Nanostructuring of templates benefits equally from top-down and bottom-up lithography approaches. The former can produce precise, arbitrary, and repetitive templates. The latter can create colloidal nanostructures through controlled solvent evaporation. This simple fabrication method enables plasmonic or light-emitting metasurfaces to characterize their spectroscopic properties. Among other applications, we demonstrate the 13-fold amplified directional radiation with an angle-resolved Fourier spectroscopy, which is the highest observed amplification factor for the perovskite-based metasurfaces. Our self-assembly process allows for the scalable fabrication of gratings with predefined periodicities and tunable chiroptical responses. We analyze our approach with numerical modeling, considering the physiochemical properties to obtain the desired geometry. This strategy makes the tunable radiative properties of such nanocrystal-based metasurfaces usable for nonlinear light-emitting devices and directional light sources.