Purpose To evaluate the performance of an artificial intelligence (AI) tool using a deep learning algorithm for detecting hemorrhage, mass effect, or hydrocephalus (HMH) at non-contrast material-enhanced head computed tomographic (CT) examinations and to determine algorithm performance for detection of suspected acute infarct (SAI). Materials and Methods This HIPAA-compliant retrospective study was completed after institutional review board approval. A training and validation dataset of noncontrast-enhanced head CT examinations that comprised 100 examinations of HMH, 22 of SAI, and 124 of noncritical findings was obtained resulting in 2583 representative images. Examinations were processed by using a convolutional neural network (deep learning) using two different window and level configurations (brain window and stroke window). AI algorithm performance was tested on a separate dataset containing 50 examinations with HMH findings, 15 with SAI findings, and 35 with noncritical findings. Results Final algorithm performance for HMH showed 90% (45 of 50) sensitivity (95% confidence interval [CI]: 78%, 97%) and 85% (68 of 80) specificity (95% CI: 76%, 92%), with area under the receiver operating characteristic curve (AUC) of 0.91 with the brain window. For SAI, the best performance was achieved with the stroke window showing 62% (13 of 21) sensitivity (95% CI: 38%, 82%) and 96% (27 of 28) specificity (95% CI: 82%, 100%), with AUC of 0.81. Conclusion AI using deep learning demonstrates promise for detecting critical findings at noncontrast-enhanced head CT. A dedicated algorithm was required to detect SAI. Detection of SAI showed lower sensitivity in comparison to detection of HMH, but showed reasonable performance. Findings support further investigation of the algorithm in a controlled and prospective clinical setting to determine whether it can independently screen noncontrast-enhanced head CT examinations and notify the interpreting radiologist of critical findings. © RSNA, 2017 Online supplemental material is available for this article.