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The taxonomic assignation and ecological implications of the genus Syringoalcyon Termier & Termier, 1945 have been a palaeontological problem for a long time. Carboniferous material from Morocco and Spain has been studied using a biomineralogical approach by means of petrographic microscopy, SEM, AFM, EMPA and CIP microscopy analysis. Detailed morphological, structural, chemical composition and crystallographic data enable a deeper understanding of the nature of Syringoalcyon. The coral walls and the so-called epithecal scales exhibit conspicuous differences in microstructure (lamellae and holacanthine fibres in the coral vs. single crystal in scales), nanostructure (pill-shaped vs. granule-shaped nanocrystals), composition (LMC vs. HMC) and crystallographic orientation. The results of these analyses imply that Syringoalcyon is an association between the tabulate coral Syringopora and an epibiont. They also suggest that the epibiont was an alcyonarian (a rare occurrence in the fossil record) that was attached to the syringoporoid. This work highlights the utility of the biomineralizational approaches for solving palaeontological problems, such as systematic affinities, and for advancing knowledge of the evolution of biocrystallization processes., (© 2015 John Wiley & Sons Ltd.)