(1) Background: Prefabricated zirconia crowns are used to restore teeth in children. The purpose of this study was to evaluate the removal of these crowns with the erbium, chromium: yttrium-scandium-gallium-garnet (Er,Cr:YSGG) laser; (2) Methods: A total of 12 primary and 12 permanent teeth were prepared and prefabricated zirconia crowns were passively fitted and cemented with two resin modified glass-ionomer (RMGI) cements. Surface areas of prepared teeth and crowns were calculated. Crowns were removed using two laser settings: 4.5 Watts, 15 Hertz, 20 water/20 air, and 5 Watts, 15 Hertz, 50 water/50 air. The retrieval time and temperature changes were tested recorded. Data were analyzed using ANOVA with Tukey's adjusted post hoc pairwise comparison -test; (3) Results: The average time for crown removal was: 3 min, 47.7 s for permanent; and 2 min 5 s for primary teeth. The mean temperature changes were 2.48 °C (SD = 1.43) for permanent; and 3.14 °C (SD = 1.88) for primary teeth. The time to debond was significantly positively correlated with tooth inner surface area and volume, outer crown volume, and the cement volume; (4) Conclusions: Use of the Er,Cr:YSGG laser is an effective, safe and non-invasive method to remove prefabricated zirconia crowns cemented with RMGI cements from permanent and primary teeth.