We report the synthesis of eight new members of the i-MAX family, of the formula (Mo2/3RE1/3)2GaC, where RE = Gd, Tb, Dy, Ho, Er, Tm, Lu, and Yb, the latter not previously incorporated in a MAX phase. The structure and composition of powder samples were investigated by X-ray diffraction, scanning transmission electron microscopy, and energy dispersive X-ray analysis combined with scanning electron microscopy. All phases showed evidence of an orthorhombic (Cmcm) structure, and the phases based on Er and Yb also crystallized in a monoclinic (C2/c) arrangement. The chemical order of the magnetic elements suggests interesting magnetic characteristics, with a high tuning potential through the range of attainable lanthanide elements.