Magnetic resonance imaging (MRI) has had a profound impact on biology and medicine. Key to its success has been the unique ability to combine imaging with nuclear magnetic resonance spectroscopy—a capability that has led to a host of powerful modalities for imaging spins. Although it remains a significant challenge, there is considerable interest to extend these powerful spectroscopic and imaging capabilities to the nanometer scale. In this talk, I will discuss a new platform for force-detected magnetic resonance detection that allows us to bring many of the tools developed for NMR to the nanometer scale. In particular, I will focus on the development of optimal control theory (OCT) pulses, which incorporate average Hamiltonian theory and realize arbitrary unitary operations. I will present initial results demonstrating the use of OCT pulses for dynamical decoupling and chemical shift averaging of nanometer scale ensembles.