Showcasing research from the Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU) GermanyUsing carbon nanodots as inexpensive and environmentally friendly sensitizers in mesoscopic solar cells Carbon nanodots (CNDs) have attracted a lot of attention due to their superior optical properties and low environmental impact. The successful incorporation of this nanomaterial in optoelectronic devices is still an open challenge however, mainly because of CNDs' heterogeneous electronic and chemical structures. A comprehensive investigation based on device characterization, spectroscopy and theory now reveals that the performance of CND solar cells is limited by a trade-off between light absorption, electronic trap states and charge regeneration kinetics.rsc.li/nanoscale-horizons Comprehensive spectroscopic and theoretical studies allow us to rationalize the nature of their absorption features. Promising power conversion efficiencies (g) of 0.24% can be achieved from these cheap and eco-friendly sensitizers by optimizing the solar-cell assembly process. Interestingly, we found that extending the light absorption towards longer wavelengths does not necessarily improve the performance of the solar cells, since the longer-wavelength absorption features hardly contribute to the cells' photo-action spectra, so that the overall power conversion efficiency is actually worse. The origin of the lower performance is corroborated in transient absorption spectroscopy and photovoltage decay measurements. Our work points, on one hand, to the limits of as-synthesized CNDs as photosensitizers and, on the other hand, to possible improvements.