Purpose: To investigate the effects of airborne-particle abrasion and nanosilica (nano-Si) infiltration treatment on the surface characteristics of dental zirconia. Materials and Methods: A total of 15 unsintered zirconia ceramic green bodies (10 × 10 × 3 mm) were divided into three groups (n = 5): Group C, no treatment after sintering; Group S, airborne-particle abrasion with 50-μm aluminum oxide particles after sintering; and Group N, infiltration of nano-Si followed by sintering and hydrofluoric acid (HF) etching. The zirconia disks’ surface roughness was analyzed by atomic force microscopy (AFM). The surface morphology of the specimens was analyzed using scanning electron microscopy (SEM), and the chemical composition was analyzed by energy-dispersive x-ray (EDX). Data were statistically analyzed by the Kruskal-Wallis test (P < .05). Results: Zirconia surface treatments by infiltration of nano-Si, sintering, and HF etching showed multiple changes in the surface features. The surface roughness of Groups C, S, and N were 0.88 ± 0.07 μm, 1.26 ± 0.10 μm, and 1.69 ± 0.15 μm, respectively. The surface roughness of Group N was significantly higher than that of Groups C and S (P < .05). EDX analysis showed peaks that corresponded to silica (Si) after infiltration with colloidal Si that disappeared following acid etching. Conclusions: Infiltrating nano-Si increases the surface roughness of zirconia. The formation of retentive nanopores on the surface potentially improves the zirconia–resin cement bonding strengths.