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Rayleigh waves are very useful for ultrasonic nondestructive evaluation of structural and mechanical components. Nonlinear Rayleigh waves have unique sensitivity to the early stages of material degradation because material nonlinearity causes distortion of the waveforms. The self-interaction of a sinusoidal waveform causes second harmonic generation, while the mutual interaction of waves creates disturbances at the sum and difference frequencies that can potentially be detected with minimal interaction with the nonlinearities in the sensing system. While the effect of surface roughness on attenuation and dispersion is well documented, its effects on the nonlinear aspects of Rayleigh wave propagation have not been investigated. Therefore, Rayleigh waves are sent along aluminum surfaces having small, but different, surface roughness values. The relative nonlinearity parameter increased significantly with surface roughness (average asperity heights 0.027–3.992 μm and Rayleigh wavelengths 0.29–1.9 mm). The relative nonlinearity parameter should be decreased by the presence of attenuation, but here it actually increased with roughness (which increases the attenuation). Thus, an attenuation-based correction was unsuccessful. Since the distortion from material nonlinearity and surface roughness occur over the same surface, it is necessary to make material nonlinearity measurements over surfaces having the same roughness or in the future develop a quantitative understanding of the roughness effect on wave distortion.