Low-dimensional materials are ideal test-beds for studying fundamental solid-state physics and hold significant promise as future platforms for technological advancement. Recent advances in both bottom-up and top-down fabrication techniques have enabled atom-by-atom modification of crystal structure and composition – generating a pantheon of new experimentally accessible nanomaterials. At the same time, the ability to elucidate the behavior of novel materials requires an incisive probe capable of reporting salient material properties concomitant with the local atomic structure. In this talk, I will highlight how state-of-the-art fabrication techniques enable rational-design of atomic-scale materials whose local electronic, magnetic, optical and plasmonic properties can be revealed using a family of scanning probes (individually and in consort). The first part of my talk will focus on one-dimensional (1D) materials known as graphene nanoribbons. I will discuss conceptual links between electronic topology and chemical bond formation, and demonstrate how these tools can be used to design tailormade 0D and 1D electronic structure. The second part of my talk will focus on graphene-based 2D heterostructures possessing significant interfacial charge transfer. I will show how the nanoscale electrostatic landscape associated with reciprocal doping of 2D layers can be interrogated by directly imaging collective light-matter excitations known as plasmon-polaritons.