This study compared the laser and rotary removals of prefabricated zirconia crowns in primary anterior and permanent posterior teeth. Sixty-two extracted teeth were prepared for prefabricated zirconia crowns cemented with resin-modified glass-ionomer cement. Specimens underwent crown removals by a rotary handpiece, or erbium, chromium: yttrium-scandium-gallium-garnet (Er,Cr:YSGG) laser. Pulpal temperatures, removal times, and scanning electron microscopy (SEM) examinations were compared. The average crown removal time for rotary and laser methods was 80.9 ± 19.36 s and 353.3 ± 110.6 s, respectively, for anterior primary teeth; and 114.2 ± 32.1 s and 288.5 ± 76.1 s, respectively, for posterior teeth (p < 0.001). The maximum temperature for the rotary and laser groups was 22.2 ± 8.5 °C and 27.7 ± 1.6 °C for anterior teeth, respectively (p < 0.001); and 21.8 ± 0.77 °C and 25.8 ± 0.85 °C for the posterior teeth, respectively (p < 0.001). More open dentinal tubules appeared in the rotary than the laser group. The rotary handpiece removal method may be more efficient than the laser with lower pulpal temperature changes. However, the laser method does not create noticeable tooth or crown structural damage compared to the rotary method.