In particular, the ease of fabrication of the active parts of these devices following solution-processing routes, such as inkjet printing, can deliver polycrystalline smooth films, with precise control over the dispensed volume. [10] Critical aspects in developing a printable device include the quality of the materials, the solution formulation, viscosity control, surface wetting to avoid solution dispersion, or long-term stability. [11,12] Specifically, viscosity is not only important for the film quality but also determines the printing technique [13] and can be divided into two main types, low viscosity or high viscosity solutions. Typically, volatile solutions do not use binders, surfactants, or other chemical additives and offer higher-purity materials. [14] However, these can affect film morphology and topography, creating the well-known "coffee-ring" effect. [15] It also presents an increased spread area with limited control of defined structures and has difficulties in controlling crystal nucleation and molecular aggregation, leading to defects, uneven thickness, and inferior device performance. [16] In this case, large and aligned crystalline domains are highly important, as they offer low charge transport anisotropy and low density of grain boundaries leading to higher optical-to-electrical conversion. [17,18] Strategies using solution-processing techniques have enabled high crystallinity organic semiconductor films. [19] However, these approaches present little or even no control on both the shape and size of the active semiconductorThe controlled growth of organic crystalline materials in predefined locations still poses a challenge for functional device application such as phototransistors, photoconductors, or photovoltaic solar cells. This work evidences the use of optical lithography and a fluoroalkylsilane to selectively modify the surface energy and how to create a wettability micro-patterned structure. These are then combined with non-contact printing of the organic solution providing custom-shaped films. To deliver printed films with improved morphological quality, key process parameters for high-performance organic materials are optimized. Particular attention is given to the adjustment of the concentration and solvent mixture to tune the jetting properties, and consequently, slow down the evaporation rate. Continuous films are obtained for an optimized number of droplets and spacing between them. Micro-Raman spectroscopy imaging confirms the crystalline nature of the printed films and the lack of impurities. To validate the method, rubrene and triisopropylsilylethynyl (TIPS)-pentacene are tested using two-terminal optoelectronic devices. TIPS-pentacene rectangular printed micrometric photosensor presents linear behavior and no hysteresis, reaching 0.33 nA under 18.1 mW cm −2 . The structural and optoelectronic characterization is in line with other micro-patterned examples, opening doors for new industrial applications.