Certain example embodiments relate to ultra-fast laser treatment of silver-inclusive (low-emissivity) low-E coatings, coated articles including such coatings, and/or associated methods. The low-E coating is formed on a substrate (e.g., borosilicate or soda lime silica glass), with the low-E coating including at least one sputter-deposited silver-based layer, and with each said silver-based layer being sandwiched between one or more dielectric layers. The low-E coating is exposed to laser pulses having a duration of no more than 10−12 seconds, a wavelength of 355-500 nm, and an energy density of more than 30 kW/cm2. The exposing is performed so as to avoid increasing temperature of the low-E coating to more than 300 degrees C. while also reducing (a) grain boundaries with respect to, and vacancies in, each said silver-based layer, (b) each said silver-based layer's refractive index, and (c) emissivity of the low-E coating compared to its as-deposited form.