The abundance and chemical composition of dissolved organic matter (DOM) in the brine of solar ponds affect the efficiency of mineral extraction and evaporation rates of the brine, and cause undesired odor and color of the products. Here, we report an investigation into the composition and changes of DOM in solar ponds from Salt Lake brine with multiple complementary analysis techniques. The results showed that the DOM derived from Salt Lake brine was primarily composed of carbohydrates, aliphatic and aromatic compounds. The concentrations of dissolved organic carbon in solar ponds increased with exposure time by up to 15−fold (from 23.4 to 330.8 mg/L) upon evaporation/irradiation of Salt Lake brine. Further qualitative analyses suggest that the relative abundance of aliphatic compounds (including functionalized ones) increased from 49.5% to 59.2% in the solar pond process, while the opposite was observed for carboxylic acid moieties, aromatics and carbohydrates, which decreased from 15.7%, 7.1% and 26.1% to 13.4%, 5.3% and 23.0%, respectively. The pyrolysis–gas chromatography–mass spectrometry results reveal that the presence of some sulfur-containing organics implied some anaerobic biotic decay, but microbiological processes were probably subordinate to photo-induced DOM transformations. In the Salt Lake brine, exposure-driven decay decreased the abundance of polysaccharides and increased that of mono- and polyaromatic pyrolysis products. Our results here provide new insights for better understanding the changes of DOM chemical composition in the solar ponds of Salt Lake brine.