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Here we present an environmental magnetic study of atmospheric deposition collected by a multi-site network in Spain that covers fourteen locations representative of urban, industrial, agricultural, and natural environments across southwestern Europe. We have combined magnetic methods with scanning electron microscopy and geochemical data to characterize the magnetic mineral assemblages of particulate matter across different types of sites and phenomenological scenarios, and to unravel their environmental significance in terms of the most important anthropogenic and natural components of atmospheric deposition. Our results enable identification of two magnetite/maghemite components of anthropogenic origin, derived mostly from vehicular traffic, plus a hematite component associated with a baseline supply of north African dust, in all the studied sites regardless of their type. The ubiquitous presence of anthropogenic magnetite/maghemite particles in pristine natural environments, albeit in lower concentrations, point to their arrival from neighbouring urban areas through atmospheric mixing processes. Samples including particulate matter deposited during distinctively intense periods of north African dust supply are characterized by a fourth component, represented also by coarser-grained hematite, that is likely derived from a different source area within the Sahara Desert. The concomitant increase observed in these cases in the amounts of magnetite/maghemite particles suggests strongly that part of the magnetite/maghemite load attributed to anthropogenic sources for the rest of the phenomenological scenarios is aeolian in origin. This seems to explain the overall moderate correlation observed between magnetite/maghemite contents and proxies for vehicular traffic, and demonstrates the need for caution when interpreting environmental magnetic proxies for magnetite/maghemite abundances in terms of anthropogenic loads. This is especially the case in southern European cities where a steady supply of north African dust occurs throughout most of the year. Our results show a good correlation between hematite abundances and geochemical proxies for north African dust, which collectively delineate broad maxima during the summer and large peaks during distinctive dust breakouts. Thus, environmental magnetic proxies of hematite abundances can be used to monitor the contribution of natural sources to atmospheric deposition. • Magnetic characterisation of atmospheric deposition in a multi-site network in Spain. • 15 sites typifying urban, industrial, agricultural and natural areas of SW Europe. • Magnetite/maghemite of anthropogenic origin occurs at all sites. • Aeolian hematite is a reliable proxy for the supply of North African dust. • Aeolian magnetite/maghemite weakens the use of these minerals as a pollution proxy. [ABSTRACT FROM AUTHOR]