The gabbro-dioritoid rocks from Veľké Železné (Nízke Tatry Mts., Western Carpathians, Slovakia) were recently studied in order to better understand the age, origin, and evolution of the basic/intermediate magmas associated with Variscan granitic rocks. Their genesis was investigated from the points of view of petrology, whole-rock geochemistry (including Sr, Nd, and Pb isotopic characteristics), as well as U–Th–Pb zircon and apatite dating. The Famennian magmatic crystallization age of ca. 360 Ma (determined from zircon: 362.4 ± 2.9 Ma and apatite: 358.4 ± 2.8 Ma) is older than the Tournaisian–Visean ages for granite intrusions in the Tatric Unit. Geochemically, the studied rocks have an affinity to arc-related basalts, consisting of a metaluminous, magnesian, and high-potassium calc-alkaline character. Isotope data (i.e., (⁸⁷Sr/⁸⁶Sr)360 = 0.7035−0.7044 and εNd360 = +1.4 to +1.6) demonstrate that these gabbro-dioritoids were formed from the mantle-influenced, lower crustal and/or sub-continental lithospheric mantle (SCLM) sources, whereas the unsystematic increase of Pb isotope ratios indicate either the melting of an ancient Enriched mantle-II (EM-II) reservoir or the upper crustal assimilation and/or local fluid alteration. The data presented in this paper favour the origin of the studied gabbro-dioritoids at a continental arc, although we cannot rule out their genesis as a result of the subsequent slab break-off.