Plasma processing is a ubiquitous surface modification technology due to its unique combination of energetic, reactive ions coupled with reactive radicals. Plasmas have proven remarkably versatile environments to controllably alter surfaces at near-room temperature and over impressively large areas. As critical dimensions continue to decrease well into the nanometer region, plasma etching will be challenged as never before. Control of plasma-surface interactions at the atomistic level will become increasingly viewed as an everyday engineering challenge, and the development of computational and experimental tools to understand and control the complex plasma will be needed. In this talk, I will present a summary of recent work in which molecular dynamics simulations of ion-surface and radical-surface interactions are combined with controlled beam experiments to develop this expertise.