This paper discusses the rheology of complex interfaces comprised of amphiphilic materials that are susceptible to flow-induced orientation and deformation. The consequence of the coupling of the film microstructure to flow leads to nonlinear rheology and surface fluid dynamics. Experimental methods designed to determine the mechanical rheological material functions of fluid-fluid interfaces as well as local, molecular and morphological responses are presented. These include a newly developed interfacial stress rheometer, flow ultraviolet dichroism, and Brewster-angle microscopy. These techniques are applied to a number of complex interfaces ranging from low molecular weight amphiphiles to polymer monolayers. Nonlinear flow phenomena ranging from two-dimensional nematic responses to highly elastic surface flows that manifest surface normal stress differences and elongational viscosities are described.