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Bottom-up nanomaterial fabrication enables control over nano building-block structure and structure-property relationships, affording opportunities to engineer devices and materials with desirable electronic and optoelectronic behaviors. Here, the authors produce stable oligophenylene dithiol cross-linked gold nanoparticle nanosheets via interfacial self-assembly and show the emergent effects of the cross-linkers on the material’s electronic, optical and photoconducting properties.