Nature Communications, Published online: 08 June 2026; doi:10.1038/s41467-026-74019-7 The authors demonstrate that N-face AlN substrate induces layer-number-parity-dependent magnetic multistates in CrI3. 5L-CrI3/AlN evolves through distinct magnetic multistates (+ 5 → –1 → +1 → –5); first-principles calculations attribute this effect to interfacial hole doping.