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Ultrasonic is one of the well-known methods for surface roughness measurement, but small roughness will only lead to a subtle variation of transmission or reflection. To explore sensitive techniques for surfaces with small roughness, nonlinear ultrasonic measurement in through-transmission and pulse-echo modes was proposed and studied based on an effective unit-cell finite element (FE) model. Higher harmonic generation in solids was realized by applying the Murnaghan hyperelastic material model. This FE model was verified by comparing the absolute value of the nonlinearity parameter with the analytical solution. Then, random surfaces with different roughness values ranging from 0 μm to 200 μm were repeatedly generated and studied in the two modes. The through-transmission mode is very suitable to measure the surfaces with roughness as small as 3% of the wavelength. The pulse-echo mode is sensitive and effective to measure the surface roughness ranging from 0.78% to 5.47% of the wavelength. This study offers a potential nondestructive testing and monitoring method for the interfaces or inner surfaces of the in-service structures. [ABSTRACT FROM AUTHOR]