In this paper, we describe the use of various methods of one-dimensional spectral compression by variable selection as well as principal component analysis (PCA) for compressing multi-dimensional sets of spectral data. We have examined methods of variable selection such as wavelength spacing, spectral derivatives, and spectral integration error. After variable selection, reduced transmission spectra must be decompressed for use. Here we examine various methods of interpolation, e.g., linear, cubic spline and piecewise cubic Hermite interpolating polynomial (PCHIP) to recover the spectra prior to estimating at-sensor radiance. Finally, we compressed multi-dimensional sets of spectral transmittance data from moderate resolution atmospheric transmission (MODTRAN) data using PCA. PCA seeks to find a set of basis spectra (vectors) that model the variance of a data matrix in a linear additive sense. Although MODTRAN data are intricate and are used in nonlinear modeling, their base spectra can be reasonably modeled using PCA yielding excellent results in terms of spectral reconstruction and estimation of at-sensor radiance. The major finding of this work is that PCA can be implemented to compress MODTRAN data with great effect, reducing file size, access time and computational burden while producing high-quality transmission spectra for a given set of input conditions.