Characterizing the bulk atmosphere of a terrestrial planet is important for determining surface pressure and potential habitability. Molecular nitrogen (N 2) constitutes the largest fraction of Earth's atmosphere and is likely to be a major constituent of many terrestrial exoplanet atmospheres. Due to its lack of significant absorption features, N 2 is extremely difficult to remotely detect. However, N 2 produces an N 2-N 2 collisional pair, (N 2) 2 , which is spectrally active. Here we report the detection of (N 2) 2 in Earth's disk-integrated spectrum. By comparing spectra from NASA's EPOXI mission to synthetic spectra from the NASA Astrobiology Institute's Virtual Planetary Laboratory three-dimensional spectral Earth model, we find that (N 2) 2 absorption produces a ~35% decrease in flux at 4.15 µm. Quantifying N 2 could provide a means of determining bulk atmospheric composition for terrestrial exoplanets and could rule out abiotic O 2 generation, which is possible in rarefied atmospheres. To explore the potential effects of (N 2) 2 in exoplanet spectra, we used radiative transfer models to generate synthetic emission and transit transmission spectra of self-consistent N 2-CO 2-H 2 O atmospheres, and analytic N 2-H 2 and N 2-H 2-CO 2 atmospheres. We show that (N 2) 2 absorption in the wings of the 4.3 µm CO 2 band is strongly dependent on N 2 partial pressures above 0.5 bar and can significantly widen this band in thick N 2 atmospheres. The (N 2) 2 transit transmission signal is up to 10 ppm for an Earth-size planet with an N 2-dominated atmosphere orbiting within the HZ of an M5V star and could be substantially larger for planets with significant H 2 mixing ratios.