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A K–Rb–<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msup><mrow></mrow><mn>83</mn></msup></semantics></math></inline-formula>Kr-based atomic comagnetometer for performing movement-related Magnetoencephalography (MEG) is theoretically studied in this paper. Parameters such as the spin-exchange rates, the spin-dephasing rates and the polarization of the nuclear spins are studied to configure the comagnetometer. The results show that the nuclear spin can generate a magnetic field of around 700 nT, at which the nuclear spin can compensate for a wide range of magnetic fields. In this paper, we also show the fabrication process for hybrid optical-pumping vapor cells, whereby alkali metals are mixed in a glove box that is then connected to the alkali vapor-cell fabrication system.