Dawsonite-type compounds, with the general formula MAlCO3(OH)(2), where M = Na+, K+, or NH4+, recently have become attractive materials because of their potential interest in geochemical CO2 sequestration, CO2 capture in power plants, and heterogeneous catalysis. However, the number of studies assessing the properties of these materials is limited. In the present paper, we report a theoretical reevaluation of the structural and essential physicochemical properties of Na-, K-, and NH4-dawsonites as determined by density functional theory (DFT) investigations. The calculated structure of Na- and K-dawsonites is in good agreement with previous data, while for NH4AlCO3(OH)(2), the calculations suggest orientation disorder of the ammonium ions in the structure. The normal-mode analysis, electronic and bonding properties, and elastic properties are reported for the three analogue dawsonites. The calculated formation enthalpy is -1714, -1699, and -1655 kJ/mol for K-, Na-, and NH4-dawsonite, respectively. This study comprises a first step toward a better understanding of the diversity of dawsonite intrinsic properties, which is required to tune their practical applications.