Pairs of correlated particles are at the core of complex many-body phenomena and their control is essential for quantum technologies. Engineering pairs that are simultaneously correlated in their external and internal degrees of freedom is a major challenge. In this work, we experimentally demonstrate a mechanism for generating pairs of atoms in well-defined spin and momentum modes. This mechanism couples atoms from a degenerate Bose gas via a superradiant photon-exchange process mediated by the vacuum mode of an optical cavity. The scheme is independent of collisional interactions, fast and tunable. We observe a collectively enhanced production of pairs, characterize their statistics, and measure inter-spin correlations in momentum space. Our observation of coherent many-body oscillations involving well-defined momentum modes offers promising prospects for quantum-enhanced interferometry using entangled matter waves.