Control of surface roughness in optical applications can have a large impact on haze. This work compares surface roughness and haze for self-assembled experimental surface structures as well as simulated surface structures for ultrathin nanocomposite films. Ultrathin nanocomposite films were synthesized from an acrylate monomer as the continuous phase with monodisperse or bidisperse mixtures of silica nanoparticles as the dispersed phase. An in-house spin coating deposition technique was used to make thin nanocomposite films on hydrophilic (glass) and hydrophobic (polycarbonate) substrates. Manipulating the size ratios of the silica nanoparticle mixtures generated multimodal height distributions, varied the average surface roughness (sigma) and changed lateral height-height correlations (a). For the simulated surfaces, roughness was estimated from their morphologies, and haze was calculated using simplified Rayleigh scattering theory. Experimental data for haze and morphologies of nanocomposite films corresponded well to these properties for simulated tipped pyramid surfaces. A correlation based on simple Rayleigh scattering theory described our experimental data well, but the exponent on the parameter, sigma/lambda (lambda is the wavelength of incident light), does not have the expected value of 2. A scalar scattering model and a prior Monte Carlo simulation estimated haze values similar to those of our experimental samples. (C) 2013 Elsevier B.V. All rights reserved.