Quantitative ultrasound techniques based on the parametrization of the backscatter coefficient (BSC) are used to characterize concentrated particle suspensions. Specifically, a scattering model is fit to the measured BSC and the fit parameters can provide local suspension properties. The scattering models generally assume an isotropic microstructure (i.e., spatial organization) of the scatterers, whereas the sheared concentrated suspensions can develop an anisotropic microstructure. This paper studied the influence of the shear-induced anisotropic microstructure of concentrated suspensions on the ultrasonic backscattering. Experiments were conducted on suspensions of polymethylmetacrylate spheres (5.8 μm in radius) sheared in a Couette flow device to obtain anisotropic microstructure and then mixed by hand to obtain isotropic microstructure. Experimental structure factors that are related to the spatial distribution of sphere positions were obtained by comparing the BSCs of one concentrated and one diluted suspension. Finally, Stokesian dynamics numerical simulations of sheared concentrated suspensions are used to determine the pair correlation function, which is linked to the Fourier transform of the structure factor. The experimental structure factors are found to be in good agreement with numerical simulations. The numerical simulation demonstrates that the angular-dependent BSCs and structure factors are caused by the shear-induced anisotropic microstructure within the suspension.