Nanoparticle-molecule arrays are a versatile mesoscale platform for investigating charge transport in artificial solids, with applications in molecular sensing, thermoelectrics, and photovoltaics. Experimentally, chemical synthesis and interfacial self-assembly enable a variety of structural and molecular configurations for these monolayer films. Comparison of experimental conductivity with simulations of hopping and tunneling charge transport in 2D networks allows analysis of the expected effects of particle polydispersity, molecular length, array crystallinity, tunneling barrier heights, and mesoscale structural defects on conductivity in these promising systems.