The accurate spectroscopic parameters reported in this work, including equilibrium rotational constants and dipole moments, are essential for guiding observational searches for these molecules. Molecules with high dipole moments, such as CH 2 NCHO and NHCHCHO, exhibit enhanced detectability through microwave spectral line analysis. The presence of stable, low-energy conformers further supports the likelihood of detecting these molecules under interstellar conditions. For example, N -methyleneformamide (1) and imine acetaldehyde (2) have favorable thermodynamic and spectroscopic properties that make them strong candidates for future observations. This study highlights the value of integrating computational methods with astrophysical observations to unravel the chemical complexity of interstellar environments. The findings highlight the role of small organic molecules in understanding the origins of chemical diversity in space. By focusing on molecules that exhibit prebiotic relevance, this study contributes to the broader effort of exploring possible connections between astrochemistry and the origins of life.