Résumé : This feature article is focused on the application of secondary ion mass spectrometry (time-of-flight SIMS) to the chemical and structural study of plasma-treated organic surfaces and plasma polymer films. After a brief historical perspective and a presentation of the recent developments of SIMS, illustrative case studies involving plasma-treated polymer surfaces and plasma polymers are presented. Beyond surface analysis by static SIMS, we show the potential of molecular depth-profiling by low-energy Cs+ ions and large Arn+ clusters for the in-depth chemical characterization of plasma-modified samples. Together with SIMS data processing by multivariate analysis, molecular depth-profiling could provide a step change for the analysis of films treated or polymerized with plasmas.