Despite their attractive features, thermoelectrics remains a niche field due to the low conversion efficiency of devices due, in part, to the challenge in overcoming the disadvantages from the interrelation between electric and thermal properties. Nevertheless, advances in computational modeling capabilities have led to new developments by combining experimental and theoretical efforts. In all this progress, materials research for lower temperatures, e.g. in cooling or refrigeration applications, does not seem to be as much of an interest as materials for higher temperature, or power generation, applications. Furthermore, developing a fundamental understanding of the underlying physical properties of materials is often secondary to thermoelectric enhancement efforts. Here I present some of our recent progress on the structure-property relationships of specific materials, provide insight into the search for new materials, and present results that demonstrate strong electron-phonon coupling and atypical transport of new layered chalcogenide materials.