The objective of this study was to assess the effect of airborne-particle abrasion with alumina particles of various sizes (50 μm, 110 μm, 250 μm) on the surface properties of 3Y-TZP (3 mol% yttria-stabilized tetragonal zirconia polycrystals). The analysis comprised the Vickers hardness test (HV1kp), a surface roughness evaluation (Ra, Rq, Rz, Rsk, Rsm, Rt, Vo, profile displays), and SEM–EDS microanalysis (scanning electron microscopy–energy-dispersive X-ray spectroscopy). Any statistical relationships were assessed using the Kruskal–Wallis one-way analysis-of-variance-by-rank test (p = 0.05). While airborne-particle abrasion with 50 µm alumina significantly increases the Vickers hardness of 3Y-TZP (1678.8 HV1kp), 110 μm and 250 μm alumina particles do not appear to have any such effect. The surface roughness of 3Y-TZP increases with the size of the alumina particles (Ra, Rq, Rz, Rt, Vo: vertical plane and retention volume assessment); a higher Rsm (horizontal plane assessment) was noted for specimens air-abraded with 250 µm alumina particles; air abrasion with 50 μm alumina particles yielded a symmetrical surface roughness profile (Rsk). The major topographic pattern of the surface of 3Y-TZP is altered by alumina airborne-particle abrasion, with larger alumina particles causing more severe changes. Aluminum traces on the 3Y-TZP surface are observed. The shape of the alumina particles is irregular, with rough edges; the size of the alumina particles plays a significant role in the air abrasion of zirconia-based dental ceramics, affecting their morphology and properties.