Bilayer or few-layer TMD materials used for applications11–13and fundamental studies14–20 are mainly derived throughmicromechanical exfoliation, limited by low yield, poor controllabilityin layer number and size. Post-treatment using laser21,plasma22,23, patterning method24, and thermal annealing25 alsoproduces few-layer, bilayer, and monolayer flakes but show sameconstrains. Contrary to these top-down methods, the bottom-upchemical vapor deposition (CVD) approach is highly regardedas one of the most promising ways to produce TMD multilayers26–29. However, the as-produced TMD structures are typicallypolycrystalline with the many randomly oriented domainsand domain boundaries, which inevitably diminish their deviceperformance29–33. Other common issues include co-existence ofareas with monolayer, bilayer, trilayer and few-layer structures,small crystal size (typically in the 10–30 μm range), and lowprocess yield26,34.