Scanning probe instruments have expanded beyond their traditional role as imaging or "reading" tools and are now routinely used for "writing." Although a variety of scanning probe lithography techniques are available, each one imposes different requirements on the types of probes that must be used. Additionally, throughput is a major concern for serial writing techniques, so for a scanning probe lithography technique to become widely applied, there needs to be a reasonable path toward a scalable architecture. Here, we use a multilayer graphene coating method to create multifunctional massively parallel probe arrays that have wear-resistant tips of uncompromised sharpness and high electrical and thermal conductivities. The optical transparency and mechanical flexibility of graphene allow this procedure to be used for coating exceptionally large, cantilever-free arrays that can pattern with electrochemical desorption and thermal, in addition to conventional, dip-pen nanolithography.scanning probe microscopy | tip modification | energy delivery | tip wear | friction T he ability to prepare nanoscale structures with the tip of a scanning probe has stimulated intense research efforts to use the scanning probe microscope as an instrument for nanofabrication on surfaces with high resolution, registration accuracy, and relatively low cost. These techniques rely on specific probes to enable the transfer of materials or energy from the probe to a surface: Dip-pen nanolithography (DPN) requires tips with controlled hydrophobicitiy (1-3); anodic oxidation requires electrically conductive tips (4, 5); mechanical scratching or nanografting requires rigid, wear-resistant tips (6-8); and thermal-scanning probe lithography (SPL) requires tips with integrated heaters (9). Therefore, understanding the tradeoffs inherent in using specialized SPL probes is important, especially when considering high throughput SPL techniques. A challenge common to all SPL techniques is to pattern with high throughput despite the serial nature of probe-based lithography. This has been addressed by the development of specialized systems, for example, one-(10) and two-dimensional cantilever arrays (11,12). The recent development of cantilever-free arrays provides a lowcost alternative to cantilever arrays for parallel SPL (13, 14).Recently, hard-tip, soft-spring lithography (HSL) has emerged as a technique for patterning sub-50-nm features over centimeter scales (15) by using an array of silicon tips resting on a compliant polydimethylsiloxane (PDMS) layer. These arrays are well suited for printing organic and inorganic structures in a high throughput and combinatorial fashion, but the versatility of these arrays is limited by the low electrical and thermal conductivities of PDMS. The adaptation of the cantilever-free architecture to additional SPL modalities would be powerful, but only lowtemperature processing steps that do not compromise the transparency and compliance of the PDMS layer can be considered. Considerable research has focused on improvi...