We explore the use of machine learning techniques to remove the response of large volume γ-ray detectors from experimental spectra. Segmented γ-ray total absorption spectrometers (TAS) allow for the simultaneous measurement of individual γ-ray energy (E γ ) and total excitation energy (E x ). Analysis of TAS detector data is complicated by the fact that the E x and E γ quantities are correlated, and therefore, techniques that simply unfold using E x and E γ response functions independently are not as accurate. In this work, we investigate the use of conditional generative adversarial networks (cGANs) to simultaneously unfold E x and E γ data in TAS detectors. Specifically, we employ a Pix2Pix cGAN, a generative modeling technique based on recent advances in deep learning, to treat (E x , E γ ) matrix unfolding as an image-to-image translation problem. We present results for simulated and experimental matrices of single-γ and double-γ decay cascades. Our model demonstrates characterization capabilities within detector resolution limits for upwards of 90% of simulated test cases.