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Two‐dimensional (2D) materials are widely used in numerous optoelectronic devices due to their ultra‐thin dimensions and versatile surfaces. However, less attention is paid to distinguishing the light‐matter interactions along the vertical and horizontal paths within the same 2D lattice, as well as comparatively investigating the optoelectronic behaviors between the sensitive top and bottom surfaces. Here, a dual‐crossbar configured architecture is designed and constructed based on Bi2O2Se semiconductor, featuring highly compact three‐in‐one assembly, namely bottom surface horizontal (BSH), middle sandwich vertical (MSV) and top surface horizontal (TSH) devices. The MSV with nanoscale channel possesses efficient separation and transportation of the photogenerated electrons and holes, responding faster to the light stimulation and compared favorably to the BSH and TSH devices. The optoelectric behaviors of the BSH device can be regulated by the characteristics of the substrate due to closer contact. Nevertheless, the performance of the TSH device is more sensitive to the environment, such as dopant absorption and heat dispersion, thus enabling the non‐volatile photoresponse and can be employed as an artificial optoelectronic synapse. This work highlights the importance of designing the device architecture based on the intrinsic structural advantages of 2D materials, paving the way toward integrated optoelectronics. [ABSTRACT FROM AUTHOR]

In this study, a detector is developed using deuterated L‐alanine doped triglycine sulfate (DLATGS) crystals capable of detecting circularly polarized light (CPL) and various polarization states. As a primary pyroelectric detection crystal, DLATGS has exhibited notable optical responses to both linearly and circularly polarized light during the tests, demonstrating a favorable polarization ratio of 3.86 and an anisotropic factor glph${g}_{lph}$ of 0.529. The research discovers the broad‐spectrum bulk photovoltaic (BPVE) characteristics in DLATGS, highlighting its potential for CPL detection. By integrating linear and circular bulk photovoltaic effect theories (LBPV and CBPV), the crystal's ability to differentiate between various polarization modes, including left‐/right‐handed polarized light, is confirmed. The BPVE and pyro‐phototronic coupling responses is characterized, laying a theoretical foundation for a rare pyroelectric effect‐based multifunctional polarization detector. The overall consistency of phenomena and theoretical framework bridges the gap between theoretical predictions and experimental validation. This work not only advances the understanding of DLATGS crystals but also sets the stage for further exploration into chiral materials and the development of TGS‐type crystals in future photoelectronic detectors. [ABSTRACT FROM AUTHOR]