In the last decade, there has been a rapid growth in research on the wavelength-scale design of materials to control optical information. Photonic crystal microcavities allow the trapping of optical fields in near fundamentally-small volumes, with many diverse applications such as filtering and switching. To effect conditional operations in a microcavity-based device, the nonlinear optical properties of multi-mode microcavities must be explored, and this theme forms the focus of this book. A resonant scattering technique is developed to si-multaneously excite multiple microcavity modes with a short-pulse laser. Using this method, the second-order nonlinear properties of InP-based microcavities are investigated, revealing sum-frequency mixing between two modes. An ultrafast pump-probe experiment is then described which demonstrates all-optical switching and frequency conversion in a silicon microcavity. This book should be a significant resource for experimentalists in the nanophotonics community, as it contains comprehensive chapters discussing each of the techniques of sample nanofabrication, numeri-cal modeling, and optical spectroscopy that are instrumental to this work.