In this overview, we discuss theoretical and experimental aspects of nonlinear two-dimensional infrared (2D-IR) spectroscopy. With this technique both peptide conformation and conformational flexibility can be probed. The quantitative relation between the experimental 2D-IR spectrum and the peptide conformation is discussed, and examples of how the conformation of a peptide and the timescale of its fluctuations are derived from its (time-resolved) 2D spectrum are presented.