Hybrid organic-inorganic perovskites (HOIPs) have emerged as promising supplies for optoelectronic purposes, but gaining management over their structural and digital tunability stays a key problem. On this examine, we introduce 7H-dibenzo[c,g]carbazole (DBCz) as a novel electroactive natural cation that permits the formation of two distinct low-dimensional hybrid steel halides: a standard 2D perovskite construction, (DBCz)2PbI4, and a beforehand unreported layered perovskite analogue construction with edge-sharing octahedra, DBCzPbI3. The sting-sharing section represents a brand new structural motif throughout the hybrid steel halide household. Each supplies exhibit a type-II band alignment, facilitating ultrafast photoinduced gap switch from the inorganic to the natural layer. Utilizing transient absorption spectroscopy, we establish the formation of DBCz-based gap polarons in each phases, and uniquely observe the charge-transfer-induced formation of triplet states and room temperature coherent phonons for the perovskite analogue section. These findings spotlight the function of molecular design in controlling excited-state dynamics and exciton-lattice interactions in hybrid steel halides.