Deep learning offers potential for various healthcare applications involving the human skull but requires extensive datasets of curated medical images. To overcome this challenge, we propose SkullGAN, a generative adversarial network (GAN), to create large datasets of synthetic skull CT slices, reducing reliance on real images and accelerating the integration of machine learning into healthcare. In our method, CT slices of 38 subjects were fed to SkullGAN, a neural network comprising over 200 million parameters. The synthetic skull images generated were evaluated based on three quantitative radiological features: skull density ratio (SDR), mean thickness, and mean intensity. They were further analyzed using t-distributed stochastic neighbor embedding (t-SNE) and by applying the SkullGAN discriminator as a classifier. The results showed that SkullGAN-generated images demonstrated similar key quantitative radiological features to real skulls. Further definitive analysis was undertaken by applying the discriminator of SkullGAN, where the SkullGAN discriminator classified 56.5% of a test set of real skull images and 55.9% of the SkullGAN-generated images as reals (the theoretical optimum being 50%), demonstrating that the SkullGAN-generated skull set is indistinguishable from the real skull set - within the limits of our nonlinear classifier. Therefore, SkullGAN makes it possible to generate large numbers of synthetic skull CT segments, necessary for training neural networks for medical applications involving the human skull. This mitigates challenges associated with preparing large, high-quality training datasets, such as access, capital, time, and the need for domain expertise.