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Diamond quantum processors consisting of a nitrogen-vacancy centre and surrounding nuclear spins have been the key to significant advancements in room-temperature quantum computing, quantum sensing and microscopy. The optimisation of these processors is crucial for the development of large-scale diamond quantum computers and the next generation of enhanced quantum sensors and microscopes. Here, we present a full model of multi-qubit diamond quantum processors and develop a semi-analytical method for designing gate pulses. This method optimises gate speed and fidelity in the presence of random control errors and is readily compatible with feedback optimisation routines. We theoretically demonstrate infidelities approaching ∼10−5 for single-qubit gates and established evidence that this can also be achieved for a two-qubit CZ gate. Consequently, our method reduces the effects of control errors below the errors introduced by hyperfine field misalignment and the unavoidable decoherence that is intrinsic to the processors. Having developed this optimal control, we simulated the performance of a diamond quantum processor by computing quantum Fourier transforms. We find that the simulated diamond quantum processor is able to achieve fast operations with low error probability. [ABSTRACT FROM AUTHOR]