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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]