Combinatorial synthesis has emerged as a highly efficient way for the pharmaceutical industry to identify new lead compounds. Recent advances in laser-induced forward transfer (LIFT) show its potential to dramatically miniaturize reaction volumes and precisely deliver different chemical agents in desired positions on a surface, which are crucial steps for combinatorial synthesis. However, the types of molecules which can be delivered by LIFT are limited, resulting in biomolecule microarrays as the core application of LIFT in chemistry. In this thesis, standard polymer-assisted LIFT (polyLIFT) has been further developed to now enable the transfer of a wide scope of materials. More importantly, new applications for this advanced polyLIFT method have been discovered for direct laser-based in-situ synthesis. The fundamental principles established in this thesis will guide laser-based molecule transfer and synthesis. The presented approach will further encourage the use of direct-writing techniques in diverse research fields, such as materials science and organic chemistry.