Simulated nanoparticle superlattices, generated with tunable defect concentrations via controlled area compression rates (mimicking the controlled evaporation rates in evaporative assembly), feature strong spatial correlations among like-resonating particles (Figure ). With a high number of defects (i.e., low values of the global hexatic order parameter Ψ 6 = 0.66, 0.79), red low-frequency resonators are found in regions with high local hexatic order, while blue high-frequency resonators are found near defective regions. In superlattices with high global order (Ψ 6 = 0.95) nearly all particles in the bulk crystalline regions resonate at the ensemble average frequency (white resonators), while red and blue resonators alike are confined to the disordered grain boundaries between bulk crystalline domains.