Deterministic processing is critical to modern precision optics finishing. Put simply, determinism is the ability to predict an outcome before carrying out an activity. With the availability of computer numerically controlled (CNC) equipment and sophisticated software algorithms, it is now possible to grind and polish optics from a variety of materials to surface shape accuracies of ~20 nm peak-to-valley (p–v), with surface roughness values (measured on white light interferometers over 250 μm×350 μm areas) to sub-nm root-mean-square (rms) levels. In the grinding phase the capability now exists to estimate removal rates, surface roughness, and the depth of subsurface damage (SSD) for a previously unprocessed material, knowing its Young's modulus, hardness, and fracture toughness. An understanding of how chemistry aids in the abrasive-driven removal of material from the surface during polishing is also critical. Recent polishing process research reveals the importance of chemistry, specifically slurry pH, for preventing particle agglomeration in order to achieve smooth surface finishes with conventional pad or pitch laps. New sub-aperture polishing processes like magnetorheological finishing (MRF) can smooth and shape flat, spherical, aspheric and free-form surfaces within a few process iterations. Difficult to finish optical materials like soft polymer polymethyl methacrylate, microstructured polycrystalline zinc sulfide, and water soluble single-crystal potassium dihydrogen phosphate (KDP) can be finished with MRF. The key is the systematic alteration of MR fluid chemistry and mechanics (i.e. the abrasive) to match the unique physical properties of each workpiece.