The increasing demand for precision optical components invokes the requirement of advanced fabrication techniques with high efficiency. Atmospheric pressure plasma processing (APPP), based on chemical etching, has a high material removal rate and a Gaussian-shaped influence function, which is suitable to generate complex structures and correct form errors. Because of the pure chemical etching, an optically smooth surface cannot be achieved using only APPP. Thus, bonnet polishing (BP) with a flexible membrane tool, also delivering a Gaussian influence-function, is introduced to smooth the surface after APPP. In this paper, the surface texture evolution in the combined process of APPP and BP is studied. The etched texture with increased removal depth of APPP is presented and analyzed. Subsequently, the processed substrates are smoothed by BP. The texture smoothing and the roughness improvement is investigated in detail. The experimental results show that the APPP etched pits coalesce with each other and transform into irregular convex-concave structures, with roughness degraded to about 25 nm arithmetical mean deviation (Ra). The APPP etched texture can be successfully smoothed to 1.5 nm Ra, with 0.2–1 μm material removal of BP.