Solid-state nuclear spins surrounding individual, optically addressable qubits provide a crucial resource for quantum networks, computation and simulation. While hosts with sparse nuclear spin baths are typically chosen to mitigate qubit decoherence, developing coherent quantum systems in nuclear spin-rich hosts enables exploration of a much broader range of materials for quantum information applications. The collective modes of these dense nuclear spin ensembles provide a natural basis for quantum storage, however, utilizing them as a resource for single spin qubits has thus far remained elusive. Here, by using a highly coherent, optically addressed 171Yb3+ qubit doped into a nuclear spin-rich yttrium orthovanadate crystal, we develop a robust quantum control protocol to manipulate the multi-level nuclear spin states of neighbouring 51V5+ lattice ions. Via a dynamically-engineered spin exchange interaction, we polarise this nuclear spin ensemble, generate collective spin excitations, and subsequently use them to implement a long-lived quantum memory. We additionally demonstrate preparation and measurement of maximally entangled 171Yb--51V Bell states. Unlike conventional, disordered nuclear spin based quantum memories, our platform is deterministic and reproducible, ensuring identical quantum registers for all 171Yb qubits. Our approach provides a framework for utilising the complex structure of dense nuclear spin baths, paving the way for building large-scale quantum networks using single rare-earth ion qubits.
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