Recent studies of Late Permian calc-alkaline lamprophyre dykes located in the Les Guilleries Paleozoic massif of the Catalan Coastal Range have revealed that allanite is present as the main REE-bearing accessory phase, which is the object of this study. The lamprophyre dykes are amphibole–plagioclase-dominated spessartites with a wide variety of accessory phases, including titanite, ilmenite, allanite, fluorapatite, spinel, zircon, and sulfides, and show complex alteration textures related to secondary albite, chlorite, epidote, titanite and calcite. The allanite crystal composition, analyzed by SEM-EPMA and LA-ICP-MS, evidences the solid solution between epidote and allanite with a ferriallanite component, similar to what is found in Variscan post-collisional granitoids from western Europe. However, heterogeneity in crystal shapes, sizes, type of zoning, dissolution embayment textures, growth of epidote coronas, mineral paragenesis, and the unique geochemical characteristics of allanite crystals suggest multiple crystallization events. At least two types of allanite–epidote composite grains have been identified: allanite Type I, with regular allanite–epidote core-to-rim zoning and a secondary allanite rim; and allanite Type II, with anhedral allanite cores surrounded by epidote coronas. Additionally, irregular zoning, complex dissolution textures and REE redistribution suggest the occurrence of deuteric and/or post-magmatic processes, which are also common in Variscan post-collisional plutons from the Catalan Coastal Range and nearby Paleozoic massifs. Multivariate statistical analyses of major elements in allanite–epidote composite grains show a relationship between major textural and geochemical variations for three out of ten principal components, mainly related to cationic substitutions between ferriallanite-(Ce) and epidote, but also involving Mn and Ti(REE3+ + Fe2+ + Ti4+ + Mg2+ + Mn2+ = Al3+ + Ca2+ + Fe3+). The allanite U-Pb-Th- weighted mean age of 265 ± 15 Ma (MSWD = 0.57) is roughly similar to the age of emplacement of the lamprophyres in the upper crust in the mid–late Permian, and coincides with the period following the main tectonometamorphic and magmatic events of the post-collisional evolution in the Catalan Coastal Range. Th/U and La/Sm ratios suggest a metamorphic origin for most allanite grains, but a combination of metamorphic processes prior to partial melting, early–late magmatic crystallization, and/or post-magmatic hydrothermal processes is the most plausible explanation to account for the diversity of allanite grains in Les Guilleries lamprophyres.