The area grown with processing potato crops in the Argentinian Pampas has been increasing steadily since 1995. The aim of this work was to assess the effects of N, P and S upon yield and tuber quality and their impact on CO2 emissions assessed with the Cool Farm Tool-Potato. During the spring-summer growing seasons 2008/2009 and 2009/2010, ten fertilization experiments to individually assess N, P and S effects were carried out in the southeast region of the Argentinian Pampas. Nitrogen (four N rates), phosphorus (four P rates) and sulfur (three S rates) were applied at planting and tuber initiation; at combined rates of 0, 50, 100 and 150 kg N ha−1, and at rates of 0, 25, 50 and 100 kg P ha−1 and 0, 10 and 20 kg S ha−1. N and P had a positive effect on total tuber yield, but tuber dry matter concentration (DMC) decreased at higher N rates. The fraction of marketable tubers suitable for processing into French fries increased with the addition of N, showed no variations with P fertilization, and decreased when S was applied. French fry colour, length/width (L:W) ratio and tuber defects were not affected by N, P and S fertilization. With regard to CO2 emissions assessed with the Cool Farm Tool-Potato, results showed that the higher the N rates the higher the CO2 emissions, but they decreased at higher yields. P and S rates did not have an impact on the CO2 emissions, which also decreased at higher yields. Under the production system of the Pampas, N should be split between planting and tuber initiation, and intermediate P rates should be applied all at planting, in order to improve crop yield and quality and to reduce CO2 emissions.