The dye-sensitized solar cell (DSSC) is one of the Most promising photovoltaic technologies with potential of low cost, light weight, and good flexibility. The practical application of DSSCs requires further improvement in power conversion efficiency and long-term stability. Recently, significant progress has been witnessed in DSSC research owing to the hovel concept of the D-A-pi-A motif for the molecular engineering of organic photosensitizers. New organic and porphyrin dyes based on the D-A-pi-A motif can not only enhance photovoltaic performance, but also improve durability in DSSC applications. This Spotlight On Applications highlights recent advances in the D-A-pi-A-based photosensitizes, specifically focusing on the mechanism of efficiency and stability enhancements. Also, we find insight into the additional acceptor as well as the trade-off of long wavelength response. The basic principles are involved in molecular engineering of efficient D-A-pi-A sensitizers, providing a clear road map showing how to modulate the energy bands, rationally extending-the response wavelength, and optimizing photovoltaic efficiency step by step.