Molecular doping of organic electronics has shown promise to sensitively modulate important device metrics. One critical challenge is the disruption of structure order upon doping of highly crystalline organic semiconductors, which significantly reduces the charge carrier mobility. This paper demonstrates a new method to achieve large modulation of charge carrier mobility via channel doping without disrupting the molecular ordering. Central to the method is the introduction of nanopores into the organic semiconductor thin films via a simple and robust templated meniscus‐guided coating method. Using this method, the charge carrier mobility of C8‐benzothieno3,2‐bbenzothiophene transistors is boosted by almost sevenfold. This paper further demonstrates enhanced electron transport by close to an order of magnitude in a diketopyrrolopyrrole‐based donor–acceptor polymer. Combining spectroscopic measurements, density functional theory calculations, and electrical characterizations, the doping mechanism is identified as partial‐charge‐transfer induced trap filling. The nanopores serve to enhance the dopant/organic semiconductor charge transfer reaction by exposing the π‐electrons to the pore wall. Doping of organic electronics without disrupting molecular packing is a critical challenge preventing effective modulation of charge‐transport properties. Enhanced charge‐transfer doping in crystalline small‐molecule and polymer transistors is reported by introducing nanopores in organic semiconductors via meniscus‐guided coating. Nanopores lead to dramatic increase in charge‐carrier mobility by promoting charge transfer reaction across the pore wall.