Levels of cocaine and other psychoactive substances in atmospheric particulate matter (PM) were determined in urban environments representing distinct social behaviours with regard to drug abuse: night-life, university and residential areas. Three cities (with population>1 million and <0.3 million inhabitants) were selected. Mean daily levels of drugs in PM were 11-336 pg/m3 for cocaine, 23-34 pg/m3 for cannabinoids, and 5-90 pg/m3 for heroin. The highest levels were recorded on weekends, with factors with respect to weekdays of 1-3 for cocaine, 1-2 for cannabinoids and 1.1-1.7 for heroin. Higher levels were detected in the night-life areas, pointing towards consumption and trafficking as major emission sources, and possibly ruling out drug manufacture. The similarities in temporal trends at all sites suggested a city-scale transport of psychoactive substances. Correlations were detected between cocaine and amphetamine consumption (r2=0.98), and between heroin and cannabinoids (r2>0.82).