Understanding the biophysics governing single-molecule transport through solid-state nanopores is of fundamental importance in working toward the goal of DNA detection and genome sequencing using nanopore-based sensors. Even with significant advances in semiconductor fabrication technologies, the state-of-the-art in nanopore technology still falls well short of mimicking the elegance and functionality found in biology. Kasianowicz et al.[1] pioneered the first in vitro studies of biomolecule transport through single nanopore channels by translocating individual ssDNA and ssRNA molecules through α-hemolysin protein pores inserted into a lipid bilayer membrane. More recently, focus has shifted to the solid-state domain with numerous groups studying biomolecule transport through solid-state nanopores.[2-7] Solid-state nanopores exhibit superior chemical, thermal, and mechanical stability over their biological counterparts, and can be fabricated using conventional semiconductor processes, thereby facilitating mass fabrication and size tunability. They are typically formed in thin Si3N4 or SiO2 membranes using a combination of decompositional ion/electron-beam-based sputtering and surface-tension-driven shrinking processes.[2,4,7] Other techniques for creating individual nanopores include the track-etch method for the formation of conical nanopores in polycarbonate membranes.[8] The translocation of negatively charged DNA molecules through these nanometer-sized solid-state pores is conventionally performed using two-terminal electrophoresis, resulting in characteristic blockades in the measured ionic current. This technique has been used to study various physical phenomena at the single-molecule level, including unzipping kinetics of hairpin DNA,[9] detection of single-nucleotide polymorphisms,[10] stretching transitions in dsDNA,[11] biomolecule folding,[3] discrimination of long DNA molecules based on length,[12] and nanopore-based DNA force spectroscopy.[13] Though this technology shows much promise, major hurdles still remain. Fabrication challenges (stress-induced membrane deformation and mechanical failure in SiO2 structures),[5] limited nanopore lifetime, electrical noise,[14,15] and a lack of chemical specificity limit the feasibility of this technology in high-end applications such as DNA sequencing. Thus, there is a need for highly sensitive, mechanically robust nanopore sensors with well-defined surface-charge properties for the detection of specific biological molecules (ssDNA, dsDNA, mRNA).