This paper is Part I of an integrated experimental/modeling investigation of a procedure to coat nanofibers and core-clad nanostructures with thin-film materials using plasma-enhanced physical vapor deposition. In the experimental effort, electrospun polymer nanofibers are coated with aluminum under varying operating conditions to observe changes in the coating morphology. This procedure begins with the sputtering of the coating material from a target. This paper focuses on the sputtering process and transport of the sputtered material through the reactor. The interrelationships among the processing factors for the sputtering and transport are investigated from a detailed modeling approach that describes the salient physical and chemical phenomena. Solution strategies that couple continuum and atomistic models are used. At the continuum scale, the sheath region and the reactor dynamics near the target surface are described. At the atomic level, molecular-dynamics (MD) simulations are used to study the sputtering and deposition mechanisms. Ion kinetic energies and fluxes are passed from the continuum sheath model to the MD simulations. These simulations calculate sputtering and sticking probabilities that in turn are used to calculate parameters for the continuum reactor model. The reactor model determines the concentration field of the coating material. (c) 2005 American Institute of Physics.