<p>Knowledge of electron backscattering coefficients (BSCs) plays a critical role in various fields, such as materials science, scanning electron microscopy (SEM), and medical physics. There is a lack of data for metals such as copper (Cu) and aluminum (Al) at various thicknesses and for a wide range of electron energies. Thus, a Monte Carlo (MC) simulation was used in this study to obtain BSCs dataset for the Cu and Al of ultrathin films (50–200 Å), intermediate films (500–1500 Å), and thicker films (3000–5000 Å), providing a broad overview of how thickness alters the BSC of a material. The calculated results agree with experimental data and data (results from other MC simulations) in the literature, especially for Al, with deviations as low as 0% at 3&#xa0;keV (500 Å). However, for Cu, the Monte Carlo model overestimates the experimental BSC values at low energies, likely due to differences in electron–atom interaction approximations. The results of this study offer an available dataset for the backscattering coefficients of Cu and Al at various thicknesses, with energies ranging from 0 to 300&#xa0;keV at normal incidence. These findings address gaps in the current database and contribute to scanning electron microscopy, materials science, and medical physics, offering insights into the backscattering behavior of different materials such as Cu and Al at different thicknesses. The dataset supplements researchers with available BSC data that can be useful in medical physics and provides an important input for MC-based SEM simulations.</p>