  Reliable, clean transfer and interfacing of 2D material layers is
technologically as important as their growth. Bringing both together remains a
challenge due to the vast, interconnected parameter space. We introduce a
fast-screening descriptor approach to demonstrate holistic data-driven
optimization across the entirety of process steps for the graphene-Cu model
system. We map the crystallographic dependencies of graphene chemical vapor
deposition, interfacial Cu oxidation to decouple graphene, and its dry
delamination across inverse pole figures. Their overlay enables us to identify
hitherto unexplored (168) higher index Cu orientations as overall optimal. We
show the effective preparation of such Cu orientations via epitaxial
close-space sublimation and achieve mechanical transfer with very high yield
(>95%) and quality of graphene domains, with room-temperature electron
mobilities in the range of 40000 cm$^2$/(Vs). Our approach is readily adaptable
to other descriptors and 2D materials systems, and we discuss the opportunities
of such holistic optimization.
