Spectroscopic investigations are performed for 5‐Bromo‐1H‐indole‐carboxaldehyde by using experimental (FT‐IR, FT‐Raman) and theoretical (DFT) calculations. Vibrational assignments of the fundamental modes were assigned on the basis of Potential energy distribution (PED) calculations. Electron Localization Function (ELF) and Local Orbital Localizer (LOL) studies were performed to visualize the electron delocalization in the molecule. Frontier molecular orbitals (FMOs) and related molecular properties were computed. The electron‐hole distribution of the molecule was also computed using Multiwfn 3.3.9 software to predict the charge transfer within the molecule. The total and partial density of states (TDOS and PDOS) and also the overlap population density of states (OPDOS) spectra were simulated. UV‐Vis spectrum of the compound was also recorded. The reactive sites of the compound were studied from the MEP and Fukui function analysis. The charge delocalization and stability of the title molecule were investigated using natural bond orbital (NBO) analysis. The lung cancer activity of the title compound against p53 tumor suppressor proteins was studied using molecular docking analysis. The in‐vitro cytotoxic activity of the molecule against human pulmonary lung cancer cell lines (A549) was determined by MTT assay.