Atmospheric radiative transfer models (RTMs) simulate the light propagation in the Earth’s atmosphere. With the evolution of RTMs, their increase in complexity makes them impractical in routine processing such as atmospheric correction. To overcome their computational burden, standard practice is to interpolate a multidimensional lookup table (LUT) of prestored simulations. However, accurate interpolation relies on large LUTs, which still implies large computation times for their generation and interpolation. In recent years, emulation has been proposed as an alternative to LUT interpolation. Emulation approximates the RTM outputs by a statistical regression model trained with a low number of RTM runs. However, a concern is whether the emulator reaches sufficient accuracy for atmospheric correction. Therefore, we have performed a systematic assessment of key aspects that impact the precision of emulating MODTRAN: 1) regression algorithm; 2) training database size; 3) dimensionality reduction (DR) method and a number of components; and 4) spectral resolution. The Gaussian processes regression (GPR) was found the most accurate emulator. The principal component analysis remains a robust DR method and nearly 20 components reach sufficient precision. Based on a database of 1000 samples covering a broad range of atmospheric conditions, GPR emulators can reconstruct the simulated spectral data with relative errors below 1% for the 95th percentile. These emulators reduce the processing time from days to minutes, preserving sufficient accuracy for atmospheric correction and providing model uncertainties and derivatives. We provide a set of guidelines and tools to design and generate accurate emulators for satellite data processing applications.