The structural, thermodynamic, and dynamical properties of water adsorbed in two homochiral metal–organic frameworks (MOFs) with general formula [Zn(l-L)(X)], X = Cl and Br, and L = 3-methyl-2-(pyridin-4-ylmethylamino)butanoic acid, are investigated through molecular dynamics simulations. Water molecules establish distinct hydrogen-bonding patterns within the pores of the two MOFs, which directly correlate with the strength of the underlying framework–water interactions. In particular, at low loading, the Zn–Cl groups of [Zn(l-L)(Cl)] effectively provide a templating scaffold for the formation of one-dimensional hydrogen-bonded water chains that propagate along the MOF channels following the helicity of the framework. In contrast, the relatively weaker framework–water interactions in [Zn(l-L)(Br)] lead to less ordered water distributions inside the pores. The simulation results are in agreement with the available experimental data and provide molecular-level insights into specific hydrogen-bonding motifs ...