Diamond is a semiconductor with many superior material properties such as high breakdown field, high saturation velocity, high carrier mobilities and the highest thermal conductivity of all materials. These extreme properties, as compared to other (wide bandgap) semiconductors, make it desirable to develop single-crystalline epitaxial diamond films for electronic device and detector applications. Future diamond devices, such as power diodes, photoconductive switches and high-frequency field effect transistors, could in principle deliver outstanding performance due to diamond's excellent intrinsic properties. However, such electronic applications put severe demands on the crystalline quality of the material. Many fundamental electronic properties of diamond are still poorly understood, which severely holds back diamond-based electronic device and detector development. This problem is largely due to incomplete knowledge of the defects in the material and due to a lack of understanding of how these defects influence transport properties. Since diamond lacks a shallow dopant that is fully thermally activated at room temperature, the conventional silicon semiconductor technology cannot be transferred to diamond devices; instead, new concepts have to be developed. Some of the more promising device concepts contain thin delta-doped layers with a very high dopant concentration, which are fully activated in conjunction with undoped (intrinsic) layers where charges are transported. Thus, it is crucial to better understand transport in high-quality undoped layers with high carrier mobilities. The focus of this doctoral thesis is therefore the study of charge transport and related electronic properties of single-crystalline plasma-deposited (SC-CVD) diamond samples, in order to improve knowledge on charge creation and transport mechanisms. Fundamental characteristics such as drift mobilities, compensation ratios and average pair-creation energy were measured. Comparing them with theoretical predictions from simulations allows for verification of these models and improvement of the diamond deposition process.