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DNA-functionalized surfaces are used as biosensors in DNA microarrays and to drive the self-assembly of biological, organic, and inorganic moieties into novel materials. However, DNA surface density, length, and linker design of the surface-functionalized DNAs significantly influence the properties of DNA-driven assemblies and materials. In the Perspective on page 1563, Abhishek Singh, Hamed Eksiri, and Yaroslava G. Yingling discuss the understanding of structure and dynamics of DNA immobilized on the surfaces from the theoretical point of view. The figure represents a snapshot from atomistic molecular dynamics simulations of DNA strands on the surface.