Self-organized nanoparticle arrays from pulsed laser-induced dewetting of ultra-thin (< 20 nm), multilayer metallic films can be used to manufacture complex multifunctional surfaces that can be applied to existing technologies such as surface Raman sensing or magnetic data storage devices, but can also enable a host of new applications that are generally based on sensing, detecting or manipulating charge, electromagnetic signals, and magnetization. This presentation and accompanying poster will attempt to describe key features of pulsed laser processing at the nanoscale, outline recent progress in experiments, and formulate challenges to quantitative modeling. It will also introduce the basic nonlinear PDE model of self-organization in bilayer films. In experiments, pulsed irradiation by thousands of pulses with pulse width around 10 ns results in film dewetting into nanoparticle arrays with well-defined length scales, composition, and intricate morphologies. We used stability analyses and computations of film height dynamics to determine dependencies of these quantities on physical and process parameters. The combined experimental/theoretical exploration is a step toward predictively manufacture scalable multifunctional surfaces in new systems.