The simulation results reported here, leveraging the recently introduced MPM for computing optical properties of disordered assemblies and the experimentally motivated coarsegrained PolyPatch model, establish how binary mixtures of short and long linkers can be chosen to deliberately template structure and modulate near-and far-field optical and mechano-optical responses of plasmonic nanoparticle linker gels. By changing the composition in a blend of short and long linkers, one can assemble plasmonic networks with qualitatively different mechano-optical responses, capturing the diversity of behaviors observed in experiments and providing insights into their structural origins. This framework can be extended in future studies, and even coupled with inverse methods, 73 to design assembly of complex plasmonic gels with novel structure-dependent properties, including hierarchical networks with planet-satellite motifs or interlaced double networks. It should also prove useful for studying linker-templated compositional ordering and optical response of binary plasmonic nanoparticle gels, complementing what is known about plasmon coupling in binary nanocrystal superlattices.