Aim: To investigate the application of anterior and posterior corneal higher order aberrations (HOAs) in detecting keratoconus (KC) and suspect keratoconus (SKC). Method: This is a retrospective, case-control study which evaluated non-ectatic (normal) eyes, SKC eyes, and KC eyes. The Sirius Scheimpfug (CSO, Italy) analyzer was used to measure HOAs of the anterior and posterior corneal surfaces. Sensitivity, specificity and area under receiver operating characteristic curve (AUC) were calculated. Results: Two-hundred and twenty eyes were included in the analysis (normal n = 108, SKC n= 42, KC n= 70). Receiver operating characteristic (ROC) curve analysis revealed a high predictive ability for anterior corneal HOAs parameters: Root mean square (RMS) total corneal HOAs, RMS trefoil and RMS coma to detect keratoconus (AUC > 0.9 for all). RMS Coma (3, ±1) derived from the anterior corneal surface was the parameter with the highest ability to discriminate between suspect keratoconus and normal eyes (AUC = 0.922; cutoff > 0.2). All posterior corneal HOAs parameters were insufficient in discriminating between SKC and normal eyes (AUC < 0.8 for all). In contrast, their ability to detect KC was excellent with AUC of > 0.9 for all except RMS spherical aberrations (AUC = 0.846). Conclusion: Anterior and posterior corneal higher order aberrations can differentiate between keratoconus and normal eyes, with a high level of certainty. In suspect keratoconus disease however, only anterior corneal HOAs, and in particular coma-like aberrations, are of value. Corneal aberrometry may be of value in screening for keratoconus in populations with a high prevalence of the disease.