The CARA program has been running since 2008 by the French reference laboratory for air quality monitoring (LCSQA) and the regional monitoring networks, to gain better knowledge—at a national level—on particulate matter (PM) chemistry and its diverse origins in urban environments. It results in strong collaborations with international-level academic partners for state-of-the-art, straightforward, and robust results and methodologies within operational air quality stakeholders (and subsequently, decision makers). Here, we illustrate some of the main outputs obtained over the last decade, thanks to this program, regarding methodological aspects (both in terms of measurement techniques and data treatment procedures) as well as acquired knowledge on the predominant PM sources. Offline and online methods are used following well-suited quality assurance and quality control procedures, notably including inter-laboratory comparison exercises. Source apportionment studies are conducted using various receptor modeling approaches. Overall, the results presented herewith underline the major influences of residential wood burning (during the cold period) and road transport emissions (exhaust and non-exhaust ones, all throughout the year), as well as substantial contributions of mineral dust and primary biogenic particles (mostly during the warm period). Long-range transport phenomena, e.g., advection of secondary inorganic aerosols from the European continental sector and of Saharan dust into the French West Indies, are also discussed in this paper. Finally, we briefly address the use of stable isotope measurements (δ15N) and of various organic molecular markers for a better understanding of the origins of ammonium and of the different organic aerosol fractions, respectively.