Spectrally resolved measurements of the Earth’s reflected shortwave (RSW) and outgoing longwave radiation (OLR) at the top of the atmosphere intrinsically contain the imprints of a multitude of climate relevant parameters. Here, we review the progress made in directly using such observations to diagnose and attribute change within the Earth system over the past four decades. We show how changes associated with perturbations such as increasing greenhouse gases are expected to be manifested across the spectrum and illustrate the enhanced discriminatory power that spectral resolution provides over broadband radiation measurements. Advances in formal detection and attribution techniques and in the design of climate model evaluation exercises employing spectrally resolved data are highlighted. We illustrate how spectral observations have been used to provide insight into key climate feedback processes and quantify multi-year variability but also indicate potential barriers to further progress. Suggestions for future research priorities in this area are provided.