The exploration of molecule-based nonlinear optical (NLO) materials at the molecular level is one of the novel areas developed recently from the viewpoint of chemistry. This review summarizes some of our recent researcheson new NLO materials based on coordination compounds, which may have potential applications in optical devices. The exploration of molecule-based nonlinear optical (NLO) materials at the molecular level is one of the novel areas recently recently from the viewpoint of chemistry. This review summarizes some of our recent researches on new NLO materials based on coordination compounds, which may have potential applications in optical devices.