Two-dimensional (2D) magnetic materials provide an ideal platform for spintronics, magnetoelectrics, and numerous intriguing physical phenomena in 2D limits. Moireś uperlattices based on 2D magnets offer an avenue for controlling the spin degree of freedom and engineering magnetic properties. However, the synthesis of high-quality, large-grain, and stable 2D magnets, much less obtaining a magnetic moirésuperlattice, is still challenging. We synthesize 2D ferromagnets (trigonal Cr 5 Te 8 ) with controlled thickness and robust stability through chemical vapor deposition. Singleunit-cell-thick flakes with lateral sizes of tens of micrometers are obtained. We observe the layer-by-layer growth mode for the crystal formation in non-van der Waals Cr 5 Te 8 . The robust anomalous Hall signal confirms that Cr 5 Te 8 of varying thickness have a long-range ferromagnetic order with an out-of-plane easy axis. There is no obvious change of the Curie temperature when the thickness of Cr 5 Te 8 decreases from 52.1 to 7.2 nm. Here, we construct diverse 2D non-van der Waals/van der Waals vertical heterostructures (Cr 5 Te 8 /graphene, Cr 5 Te 8 /h-BN, Cr 5 Te 8 /MoS 2 ). A uniform moirésuperlattice is formed in the heterostructure through a lattice mismatch. The successful growth of 2D Cr 5 Te 8 and a related moirésuperlattice introduces 2D non-van der Waals ferromagnets into moirésuperlattice research, thus highlighting prospects for property investigation of a non-van der Waals magnetic moirésuperlattice and massive applications which require a scalable approach to magnetic moirésuperlattices.

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Two-dimensional (2D) magnetic heterostructures provide ideal platforms for manipulating the spin degree of freedom, exploring interfacial coupling effects, and exploiting novel spintronic devices. However, controlled synthesis of magnetic heterostructures remains challenging, especially for magnetic lateral heterostructures. Here, we synthesize magnetic lateral and vertical heterostructures via chemical vapor deposition. The lateral and vertical antiferromagnetic−ferromagnetic non-van der Waals (vdWs) α-MnSe/Cr 2 Se 3 heterostructures can be selectively attained by tuning the vapor concentrations of precursors. The lateral heterostructures manifest sharp and contaminant-free interfaces without obvious extended defects. Moreover, a non-vdWs/non-vdWs lateral heterostructure at the 2D limit (∼1 nm) is grown. The vertical heterostructures exhibit uniform and highly ordered superlattices, indicating the high quality of the moireś uperlattices. We further apply this heteroepitaxial growth approach to synthesize non-vdWs/vdWs magnetic heterostructures, including α-MnSe/graphene and α-MnSe/MoS 2 . Our work paves the way for the scalable synthesis of two-dimensional lateral and vertical magnetic heterostructures for fundamental studies and potential device applications.