Recently, polyetheretherketone (PEEK) has been introduced to the dental market as a high-performance and chemically inert biomaterial. This study aimed to compare the wear resistance, abrasiveness, color stability, and displacement resistance of zirconia and PEEK milled crowns. An ideal tooth preparation of a first maxillary molar was done and scanned by an intraoral scanner to make a digital model. Then, the prosthetic crown was digitally designed on the CAD software, and the STL file was milled in zirconia (CaroZiir S, Carol Zircolite Pvt. Ltd., Gujarat, India) and PEEK (BioHpp, Bredent GmbH, Senden, Germany) crowns using five-axis CNC milling machines. The wear resistance, color stability, and displacement resistance of the milled monolithic zirconia with unfilled PEEK crowns using a chewing simulator with thermocyclic aging (120,000 cycles) were compared. The antagonist wear, material wear, color stability, and displacement were evaluated and compared among the groups using the Wilcoxon–Mann–Whitney U-test. Zirconia was shown to be three times more abrasive than PEEK (p value < 0.05). Zirconia had twice the wear resistance of PEEK (p value < 0.05). Zirconia was more color stable than PEEK (p value < 0.05). PEEK had more displacement resistance than zirconia (p value < 0.05). PEEK offers minimal abrasion, better stress modulation through plastic deformation, and good color stability, which make it a promising alternative to zirconia crown.