We investigate theoretically the spin purity of single holes confined in vertically coupled GaAs/AlGaAs quantum dots (QDs) under longitudinal magnetic fields. A unique behavior is observed for triangular QDs, by which the spin is largely pure when the hole is in one of the dots, but it becomes strongly mixed when an electric field is used to drive it into molecular resonance. The spin admixture is due to the valence-band spin-orbit interaction, which is greatly enhanced in C 3h symmetry environments. The strong yet reversible electrical control of hole spin suggests that molecules with C 3 -symmetry QDs, like those obtained with [111] growth, can outperform the usual C 2 -symmetry QDs obtained with [001] Single spins confined in III-V semiconductor quantum dots (QDs) are currently considered as potential qubits for solid-state quantum-information processing, which combine fast optical and electrical manipulation with prospects of scalability [1][2][3][4]. In recent years, heavy-hole spin qubits have emerged as a robust and long-lived alternative to electron spins, as they can be less sensitive to dephasing from nuclear spins [1][2][3][4][5][6][7][8][9]. Significant advances have been reported on hole spin initialization, control, and readout by means of optical excitations [2-4,10-13], and different proposals for electrical control have been put forward [14][15][16][17][18].Although most works so far have focused on QDs grown along [001], it has been noted that the C 2 point symmetry of such systems gives rise to a splitting of bright exciton states that limits the fidelity of optical hole spin preparation [12,19]. No such splitting is expected, however, in [111] grown QDs due to their higher (C 3 ) symmetry [20,21], which hence become an alternative worth exploring. Early studies on single (In)GaAs/AlGaAs QDs grown along [111] have revealed that hole states have weak heavy-hole-light-hole (HH-LH) coupling due to the large aspect ratio, which is a prerequisite to obtain pure hole spins and minimize the impact of hyperfine interaction with the lattice nuclei [22]. In turn, magnetophotoluminescence spectra have reported characteristic differences from [001] grown QDs that were ascribed to the influence of the C 3 symmetry on the hole states [23].In this paper, we move forward and study hole states confined in quantum dot molecules (QDM) formed by a pair of vertically stacked QDs grown along [111]. QDMs present several advantages over single QDs for qubit development, including readout independency from initialization and measurement protocols [24], higher fidelity of spin preparation [10], and enhanced wavelength tunability with external electric fields, which greatly improves prospects of scalability [25]. We consider [111] grown GaAs/AlGaAs QDMs with a triangular shape, similar to those reported in Refs. [26,27], adding longitudinal magnetic and electric fields to control the Zeeman splitting and charge localization. Our calculations show that the HH spin purity is high when the * josep.planelles@uji.es; ...