Colloidal Nanocrystals In article number 2310671, Seung-Yong Lee, Jaeyoung Jang, Nuri Oh, and co-workers describe a synthetic strategy for colloidal p-type Zn3As2 nanocrystals from new As precursors by elucidating the formation mechanisms of Zn3As2 from precursor states. The synthesized Zn3As2 nanocrystals possess high crystallinity, are well-assembled on FET devices, and demonstrate high hole mobility.