Research into 2D layered hybrid perovskites is on the rise due to the enhanced stability of these materials compared to 3D hybrid perovskites. Recently, interest towards the use of functional organic cations for these materials is increasing. However, a vast amount of the parameter space remains unexplored in multi-layered (n > 1) hybrid perovskites for solar cell applications. Here, we incorporate carbazole derivatives as a proof of concept towards the use of tailored functional molecules in multi-layered perovskites. Films of low-n carbazole containing perovskites show high photoconductivity half-lifetimes. Higher-n (〈n〉 = 40) multi-layered perovskite films possess charge carrier diffusion lengths comparable to MAPI thin films. Solar cells containing these materials have comparable efficiencies to our MAPI and phenethylammonium (PEA)-containing multi-layered perovskite reference devices. Moisture stability tests were performed both at the material and device levels. In comparison to MAPI and PEA-based materials and solar cells, the addition of a small percentage of the carbazole derivative to the perovskite material significantly enhances the moisture stability.