In spite of its recognized potential, studies on thin film deposition of organic systems by laser ablation are so far limited in number. In this paper, experimental results of the fabrication of polymer and non-polymer organic thin films by pulsed laser ablation are described. We succeeded in fabrication of crystalline thin films of polytetrafluoroethylene (PTFE) with an F₂ laser (157 nm). In this fluoropolymer deposition, cluster formation in the ablation plume under-200 mTorr Ar ambient gas keeps the bulk composition of the target in the films. PTFE thin films containing semiconductor CdTe microcrystallites, which exhibit a 3rd-order optical nonlinearity, were also fabricated in all ablation processes. These techniques were extended to non-polymer organic materials such as copper-phthalocyanine (CuPc) and 4-dialkylamino-4-nitrostilbene (DANS).