Our understanding of the biogeochemical cycling of the climate-relevant trace gas dimethyl sulfide (DMS) in the Peruvian upwelling system is still limited. Here we present oceanic and atmospheric DMS measurements which were made during two shipborne cruises in December 2012 (M91) and October 2015 (SO243) in the Peruvian upwelling region. Dimethylsulfoniopropionate (DMSP) and dimethyl sulfoxide (DMSO) were also measured during M91. DMS concentrations were 1.9 ± 0.9 and 2.5 ± 1.9 nmol L−1 in surface waters in October 2015 and December 2012, respectively. Nutrient availability appeared to be the main driver of the observed variability in the surface DMS distributions in the coastal areas. DMS, DMSP, and DMSO showed maxima in the surface layer, and no elevated concentrations associated with the oxygen minimum zone off Peru were measured. The possible role of DMS, DMSP, and DMSO as radical scavengers (stimulated by nitrogen limitation) is supported by their negative correlations with N:P (sum of nitrate and nitrite : dissolved phosphate) ratios. Large variations in atmospheric DMS mole fractions were measured during M91 (144.6 ± 95.0 ppt) and SO243 (91.4 ± 55.8 ppt); however, the atmospheric mole fractions were generally low, and the sea-to-air flux was primarily driven by seawater DMS. The Peruvian upwelling region was identified as a source of atmospheric DMS in December 2012 and October 2015. However, in comparison to the previous measurements in the adjacent regions, the Peru upwelling was a moderate source of DMS emissions at either time (M91: 5.9 ± 5.3 µmol m−2 d−1; SO243: 3.8 ± 2.7 µmol m−2 d−1).