Judiciously matched experiments, calculations, and theory demonstrate that a higher sensitivity to short-range interactions and, consequently, improved resolution on the atomic scale can be achieved by bimodal noncontact dynamic force microscopy. The combination of sub-Angström tip oscillation at the second flexural resonance of a commercially available silicon cantilever with the commonly used large amplitude oscillation at the fundamental resonance frequency enables this performance improvement while avoiding potentially damaging jump-to-contact instabilities.