First principles modeling is a versatile tool for the molecular-level understanding of nanofabrication technologies adopted for the development of advanced functional materials and devices. In this broad scenario, a representative example is offered by chemical vapor deposition (CVD), a bottom-up route exploiting the controlled conversion of gas-phase precursor molecules into the target material. In the perspective on page 1, Gloria Tabacchi et al. exploit first principles modeling to investigate some complex and still largely unexplored steps of CVD processes. By focusing on case studies, the computational approach demonstrates its potential to open the Pandora's Jar of molecule-to-material conversion in CVD.