Golf ball comprising a core having a hardness gradient and an outer cover layer having a microhardness gradient and being formed from a thermoset polyurethane material throughout, and having: i) a treated region that is contacted with a thermoset polyurethane microhardness-increasing solution consisting of an isocyanate portion and at least one non-aqueous solvent; and ii) an untreated region that is not contacted with the thermoset polyurethane microhardness-increasing solution. The treated region comprises the isocyanate portion, whereas the untreated region does not comprise the isocyanate portion. Treated region has a microhardness M1 that is greater than microhardness M2 of untreated region to define the outer cover layer positive microhardness gradient ΔM=M1−M2. The treated region may have a depth Dtr that extends inward from the cover outer surface and in some embodiments is less than a thickness of the untreated region. Treated region may alternatively extend from the inner surface toward outer surface.