Optical metasurfaces address a plethora of applications in planar optics, as they enable precise control of the phase, amplitude, and polarization of light at nanoscale interaction lengths. However, their implementation requires surface nanostructuring, based on complex design and fabrication methods. In addition, exploiting narrow spectral features, e.g., for sensing, is accompanied by high demands in terms of precise post‐process alignments of probing light—impractical for compact optical systems. Here, the realization of plasmonic metasurfaces, based on silver nanoparticles (AgNPs) and using a solution‐based growth method, is demonstrated. The particle growth is mediated by localized surface plasmon resonances. The resulting nanostructures are directly applicable as self‐optimized metasurfaces in optical systems, as their fabrication and probing procedures allow the use of common—photonic and plasmonic—platforms. Information regarding the electromagnetic (EM) environment is stored during the fabrication via distinct particle positions and dimensions. The resulting optical response is inherently sensitive to deviations from this EM environment—enabling high‐performance nanoplasmonic sensing with a maximum discrete Figure of Merit* (FoMmax∗ of 968 without the need for post‐process alignments.