Replacing electronic components with molecule-sized analogs or hybrids is often seen as a promising alternative to further miniaturization of conventional electronics in the effort to achieve functional nanoscale circuit elements. In this thesis, electronic transport through self-assembled networks with tunable thiolated (alkane(di)thiol and benzenedithiol) molecule-to-colloidal gold (Au) nanoparticle ratios (1:5–50:1) is studied using a combination of broad area and scanning probe microscope-based measurements. The electronic transport paths through the network can be altered by adjusting the (di)thiol molecule–gold nanoparticle ratio and/or type of molecules in the network. Resistance can be controllably tuned by several orders of magnitude (~105 to 1011 ohms for the Au-thiolated structures studied). Two-terminal current–voltage (I-V) measurements of the Au-thiolated networks display linear behavior at low bias. High bias measurements in case of benzenedithiol networks show nonlinear negative differential resistance (NDR) and hysteresis behavior for different benzenedithiol concentrations, which can be attributed to a combination of field-assisted tunneling and charge trapping occurring in the nanoscale networks. Circuit simulations that account for different network morphologies, tunable via molecule-to-nanoparticle ratio, and defects show good agreement with the experiment and provide a guide to engineer network properties using different molecules. In addition, electronic transport properties of nanoscale networks, which are composed of Au metal clusters interconnected with thiolated molecules (benzene/alkanedithiol) and connected in linear chains and branched extended networks, are examined via first-principles density functional theory-based simulations. Calculated I-V characteristics of the metal-molecular networks exhibited nonlinearities and rectification with NDR peaks that became more pronounced with increasing chain length. The transmission spectra of the linear chains and branched networks showed an increase in the number and width of transmission peaks near the Fermi energy, as the structures were extended, indicating enhanced transmission. 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. These experimental and simulation results are utilized to propose molecular-scale circuits in applications such as memory, switching, and hardware security. The metal nanoparticle molecular electronic networks presented in this thesis provide an avenue for engineering electronics at the molecular level. / Graduate