Resumen: We explore how to encode more than a qubit in vanadyl porphyrin molecules hosting a S = 1/2 electronic spin coupled to a I = 7/2 nuclear spin. The spin Hamiltonian and its parameters, as well as the spin dynamics, have been determined via a combination of electron paramagnetic resonance, heat capacity, magnetization and on-chip magnetic spectroscopy experiments performed on single crystals. We find low temperature spin coherence times of micro-seconds and spin relaxation times longer than a second. For sufficiently strong magnetic fields (B > 0.1 T, corresponding to resonance frequencies of 9-10 GHz) these properties make vanadyl porphyrin molecules suitable qubit realizations. The presence of multiple equispaced nuclear spin levels then merely provides 8 alternatives to define the ''1'' and ''0'' basis states. For lower magnetic fields (B < 0.1 T), and lower frequencies (<2 GHz), we find spectroscopic signatures of a sizeable electronuclear entanglement. This effect generates a larger set of allowed transitions between different electronuclear spin states and removes their degeneracies. Under these conditions, we show that each molecule fulfills the conditions to act as a universal 4-qubit processor or, equivalently, as a d = 16 qudit. These findings widen the catalogue of chemically designed systems able to implement non-trivial quantum functionalities, such as quantum simulations and, especially, quantum error correction at the molecular level. Idioma: Inglés DOI: 10.1039/d1sc00564b Año: 2021 Publicado en: CHEMICAL SCIENCE 12, 15 (2021), 5621-5630 ISSN: 2041-6520 Factor impacto JCR: 9.969 (2021) Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 25 / 180 = 0.139 (2021) - Q1 - T1 Factor impacto SCIMAGO: 2.878 - Chemistry (miscellaneous) (Q1)