Airborne gamma-ray surveys are useful for many applications, ranging from geology and mining to public health and nuclear security. In all these contexts, the ability to decompose a measured spectrum into a linear combination of background source terms can provide useful insights into the data and lead to improvements over techniques that use spectral energy windows. Multiple methods for the linear decomposition of spectra exist but are subject to various drawbacks, such as allowing negative photon fluxes or requiring detailed Monte Carlo modeling. We propose using Non-negative Matrix Factorization (NMF) as a data-driven approach to spectral decomposition. Using aerial surveys that include flights over water, we demonstrate that the mathematical approach of NMF finds physically relevant structure in aerial gamma-ray background, namely that measured spectra can be expressed as the sum of nearby terrestrial emission, distant terrestrial emission, and radon and cosmic emission. These NMF background components are compared to the background components obtained using Noise-Adjusted Singular Value Decomposition (NASVD), which contain negative photon fluxes and thus do not represent emission spectra in as straightforward a way. Finally, we comment on potential areas of research that are enabled by NMF decompositions, such as new approaches to spectral anomaly detection and data fusion.