Machine learning (ML) is an effective tool to interrogate complex systems to find optimal parameters more efficiently than through manual methods. This efficiency is particularly important for systems with complex dynamics between multiple parameters and a subsequent high number of parameter configurations, where an exhaustive optimisation search would be impractical. Here we present a number of automated machine learning strategies utilised for optimisation of a single-beam caesium (Cs) spin exchange relaxation free (SERF) optically pumped magnetometer (OPM). The sensitivity of the OPM (T/Hz), is optimised through direct measurement of the noise floor, and indirectly through measurement of the on-resonance demodulated gradient (mV/nT) of the zero-field resonance. Both methods provide a viable strategy for the optimisation of sensitivity through effective control of the OPM’s operational parameters. Ultimately, this machine learning approach increased the optimal sensitivity from 500 fT/Hz to textless109fT/Hz. The flexibility and efficiency of the ML approaches can be utilised to benchmark SERF OPM sensor hardware improvements, such as cell geometry, alkali species and sensor topologies.