The development of current sexing methods largely depends on the use of adequate sources of data and adjustable classification techniques. Most sex estimation methods have been based on linear measurements, while the angles have been largely ignored, potentially leading to the loss of valuable information for sex discrimination. This study aims to evaluate the usefulness of cranial angles for sex estimation and to differentiate the most dimorphic ones by training machine learning algorithms. Computed tomography images of 154 males and 180 females were used to derive data of 36 cranial angles. The classification models were created by support vector machines, naïve Bayes, logistic regression, and the rule-induction algorithm CN2. A series of cranial angle subsets was arranged by an attribute selection scheme. The algorithms achieved the highest accuracy on subsets of cranial angles, most of which correspond to well-known features for sex discrimination. Angles characterizing the lower forehead and upper midface were included in the best-performing models of all algorithms. The accuracy results showed the considerable classification potential of the cranial angles. The study demonstrates the value of the cranial angles as sex indicators and the possibility to enhance the sex estimation accuracy by using them.