The surface treatment of zirconia prior to bonding remains controversial and unclear. This study aimed to compare the shear bond strength (SBS) of metal brackets to zirconia under surface treatments with either 4% HF or 37% PA in both immediate loading (IML) and artificial aging by thermocycling (TMC). Methods: Eighty-four zirconia were randomly assigned to six groups based on the surface treatment and artificial aging by TMC: (1) No surface treatment (NT); (2) NT + TMC; (3) HF (4% HF for 2 min); (4) HF + TMC; (5) PA (37% PA for 2 min); and (6) PA + TMC. After bracket bonding, only the TMC groups were thermocycled for 5000 cycles. The SBS and adhesive remnant index (ARI) of all groups were analyzed (p p p p > 0.01). Conclusions: Two-minute simple etching methods, using either 4% HF or 37% PA, showed an insufficient SBS of metal orthodontic brackets to zirconia after TMC.