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Abstract Photodetectors that can sense not only light intensity but also light's polarization state add valuable information that is beneficial in a wide array of applications. Polymer semiconductors are an attractive material system to achieve intrinsic polarization sensitivity due to their anisotropic optoelectronic properties. In this report, the thermomechanical properties of the polymer semiconductors PBnDT‐FTAZ and P(NDI2OD‐T2) are leveraged to realize bulk heterojunction (BHJ) films with record in‐plane alignment. Two polymer blends with distinct weight average molar masses (Mw) are considered and either a strain‐ or rub‐alignment process is applied to align the polymer blend films. Optimized processing yields films with dichroic ratios (DR) of over 11 for the highMwsystem and nearly 17 for the lowMwsystem. Incorporating the aligned films into photodetectors results in a polarized photocurrent ratio of 15.25 with corresponding anisotropy ratio of 0.88 at a wavelength of 530 nm, representing the highest reported photocurrent ratio for photodiodes that can operate in a self‐powered regime. The demonstrated performance showcases the ability of polymer semiconductors to achieve BHJ films with exceptional in‐plane polymer alignment, enabling high performance polarization sensitive photodetectors for incorporation into novel device architectures.