Halide perovskites have attracted significant attention as cutting-edge semiconducting materials, particularly as ultrathin layers for optoelectronic applications. However, producing these materials in a controlled way when the nature of the cation is varied, has posed numerous challenges. Herein, we explored the use of aminated silane modification for the controlled growth of perovskite nanosheets (NSs) containing bivalent conjugated cations (1,5-diaminonaphthalene) as new semiconducting materials. Surface modification implementation enabled achieving a higher degree of control over the morphology and lateral dimensions of NSs and obtaining micrometer-size particles with uniform thickness. Kelvin-probe force microscopy investigations demonstrated photo-induced charge generation, where the NSs exhibited significantly changed, and mostly reversible, surface potential under ultraviolet illumination, thereby providing proof of concept for these materials in photodetector applications.