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We describe a highly sensitive method of measuring electrophoretic mobility and zeta potential of water-dispersed colloidal particles by using a self-mixing laser Doppler velocimeter with a laser-diode-pumped, thin-slice solid-state laser with extremely high optical sensitivity. The power spectra of laser output modulated by reinjected laser light scattered by the electrophoretic particles were observed. The power spectrum cannot be described by the well-known formula for translational motion or flowing Brownian motion, i.e., a combination of Doppler shift, diffusion, and translation. The power spectra shape is found to reflect the velocity distribution of electrophoretic particles in a capillary tube due to the electro-osmotic flow contribution. Not only evaluation of the electrophoretic mobility and zeta potential but also the particle diameter undergoing electrophoretic motion can be performed from the shape of the power spectrum.