Sea surface salinity (SSS) is a major ocean circulation component and indicator of the hydrological cycle. Here we investigate an unprecedented Atlantic SSS compilation from 1896 to 2013 and analyze the main modes of SSS decadal variability. Using principal component analysis, we find that the low-latitude (tropical and subtropical) Atlantic and the subpolar Atlantic have distinct variability. Subpolar and low-latitude SSS are negatively correlated, with subpolar anomalies leading low-latitude anomalies by about a decade. Subpolar SSS varies in phase with the Atlantic Multidecadal Oscillation (AMO), whereas low-latitude SSS varies in phase with the North Atlantic Oscillation (NAO). Additionally, northern tropical SSS is anticorrelated with Sahel rainfall, suggesting that SSS reflects the Intertropical Convergence Zone latitude. The 1896–2013 SSS trend shows amplification of the mean SSS field, with subpolar freshening and low-latitude salinification. The AMO and NAO have little effect on the long-term trend but contribute to the trend since 1970.