Complementing electronic components with molecular analogs is a promising alternative to further miniaturization of conventional silicon electronic devices in the quest to achieve functional molecular nanoscale circuit elements. To this end, molecular units have been widely investigated to evaluate their suitability for future nanoelectronic circuit applications. Previous work has typically either focused on tightly packed layers of dithiol molecule-encapsulated gold nanoparticles or small oligomeric structures comprised of nanoparticles linked by a few dithiol molecules. In this thesis, we study the electrical and electronic properties of metal-molecular networks having an intermediate number of dithiol molecules both theoretically and experimentally. Electronic transport through self-assembled networks with tunable thiol molecule: gold nanoparticle ratios (ranging from 1:1 to 50:1) is studied using two-terminal electrical characterization techniques. The tunability of the electrical properties (e.g., resistance, current etc.) of the molecular networks on modifying the thiol molecule: gold nanoparticle ratios and/or type of molecule used was observed. Specifically, the current in the molecular networks studied typically decreased with increasing molecule: AuNP. For example, in gold-benzenedithiol molecular networks with approximately the same length-to-width ratios, current at low bias, 0.3 V, was found to decrease from the μA range in 1:1 ratio samples to the nA range in 50:1 samples. Additionally, many gold-benzenedithiol molecular networks which had linear I-V characteristics at low biases displayed nonlinearities in their I-Vs at higher biases. In such cases, the nonlinearities in the I-Vs at higher biases became more pronounced with increasing molecule: AuNP ratio. For example, in a control sample, consisting of only gold nanoparticles, linear I-V behaviour was observed, while the 50:1 gold-benzenedithiol molecular network displayed NDR with a measured peak-to-valley ratio of approximately 1.52. A linear resistor circuit model provided accurate approximations of the low bias I-V behaviour of the molecular networks. Experimental studies were complemented with first principles density functional theory-based simulations of the molecular networks. Linear chains and branched networks of interconnected benzenedithiol molecules and Au6 clusters were the systems of interest in this study. Calculated current-voltage characteristics of the metal-molecular networks exhibited nonlinearities and rectification with negative differential resistance (NDR) peaks that became more pronounced with increasing chain length of the linear chains. Peak-to-valley current NDR ratios as large as ~ 500 and rectification ratios of ~ 10 (0.25 V) were shown for linear and branched circuit elements, respectively, illustrating how charge transport through molecular-scale devices could be controlled with precision by modifying the structure and geometry of molecule-nanoparticle networks. Observed nonlinearities (e.g., NDR, hysteresis, and rectification) in the I-Vs of the self-assembled metal-molecular networks studied highlight their potential for application as circuit elements in future nanoelectronic devices and circuits, including memory, logic, switching and sensing. Additionally, the device level physical randomness and imperfections induced during fabrication of the metal-molecular networks, as well as the variability of the resistance of the networks on modifying the molecule: gold nanoparticle ratios can be applied for generating random binary sequences. / Graduate