In Bajo de La Leona, located in the eastern Deseado Massif, pre-Permian basement rocks of the Río Deseado Complex crop out. They consist of high- to medium-grade metamorphic rocks intruded by two Paleozoic granitoids, namely the Mina de La Leona Granite and the Laguna Larga Granite. The latter is the main goal of this work. It is a calc-alkaline to high-K calc-alkaline, ferroan, calcic to alkali-calcic, and mainly peraluminous monzoleucogranite which plots within the I&S-type and volcanic-arc fields of the tectonic discrimination diagrams. Its trace elements composition (e.g., Sr/Y, LaN/YbN, Sm/Yb, Eu/Eu*, Dy/Dy*, Dy/Yb) suggests plagioclase ± clinopyroxene fractionation in a shallow source at low pressures. Assimilation could have played a role in magma differentiation, thus the magmatic development of the Laguna Larga Granite is likely a consequence of assimilation-fractional crystallization (AFC) processes. Coupled LA-ICP-MS U–Pb and Lu–Hf zircon data for the studied granite, as well as Sm–Nd whole-rock data, are here presented for the first time. A Famennian U–Pb zircon crystallization age of 361.9 ± 1.7 Ma was obtained, together with εHf(t) zircon values from -15 to +6 with TDM-Hf model ages between 2.0 and 0.9 Ga. A thin crust, as suggested by low values of thickness proxies such as Sr/Y (1.06–1.83) and LaN/YbN (3.97–4.96), would allow emplacement of juvenile mantle-derived material, giving rise to the suprachondritic εHf(t) values. A mantle-derived source is also suggested by a suprachondritic εNd(t) whole-rock value of +2.34 (TDM-Nd = 0.93 Ga). On the other hand, the subchondritic εHf(t) values could be related to wall rock assimilation. In a regional context, the obtained results for the Laguna Larga Granite allow to correlate it with coeval rocks from northern Patagonia (e.g., San Martín de los Andes batholith, Paleozoic Central Patagonian igneous-metamorphic belt). Therefore, the Devonian magmatic arc might have extended from the North Patagonian Andes and the western North Patagonian Massif to the eastern Deseado Massif along a NNW-SSE-striking belt, confirming previous proposals.