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We report muon spin rotation ($\mu$SR) and neutron diffraction on therare-earth based magnets (Mo$_{2/3}$RE$_{1/3}$)$_2$AlC, also predicted asparent materials for 2D derivatives, where RE = Nd, Gd (only ($\mu$SR), Tb, Dy,Ho and Er. By crossing information between the two techniques, we determine themagnetic moment ($m$), structure, and dynamic properties of all compounds. Wefind that only for RE = Nd and Gd the moments are frozen on a microsecond timescale. Out of these two, the most promising compound for a potential 2D high($m$) magnet is the Gd variant, since the parent crystals are pristine with $m= 6.5 \pm 0.5 \mu_B$, N\'eel temperature of $29 \pm 1$ K, and the magneticanisotropy between in and out of plane coupling is smaller than $10^{-8}$. Thisresult suggests that magnetic ordering in the Gd variant is dominated byin-plane magnetic interactions and should therefore remain stable if exfoliatedinto 2D sheets.

Magnetic structure determination of rare-earth based, high moment, atomic laminates; potential parent materials for 2D magnets