Two substrate-biasing techniques, i.e., substrate-tuned biasing and RF biasing, have been implemented in a remote plasma configuration, enabling control of the ion energy during plasma-assisted atomic layer deposition (ALD). With both techniques, substrate bias voltages up to −200 V have been reached, which allowed for ion energies up to 272 eV. Besides the bias voltage, the ion energy and the ion flux, also the electron temperature, the electron density, and the optical emission of the plasma have been measured. The effects of substrate biasing during plasma-assisted ALD have been investigated for Al2O3, Co3O4, and TiO2 thin films. The growth per cycle, the mass density, and the crystallinity have been investigated, and it was found that these process and material properties can be tailored using substrate biasing. Additionally, the residual stress in substrates coated with Al2O3 films varied with the substrate bias voltage. The results reported in this article demonstrate that substrate biasing is a promising technique to tailor the material properties of thin films synthesized by plasma-assisted ALD.