The parameters obtained by ∂-HyMD reproduce with good accuracy the fluctuations in the difference between the normal and lateral components of the pressure, as compared to the all-atom reference, and previous gradient-free parameterization. In particular, they yield the tensionless condition for the bilater as a balance between the laterally compacting hydrophobic tails, and the laterally expanding hydrophilic heads. The good quality of the pressure profiles confirms that the parameters obtained by this optimization procedure describe well the physics of the system, and can be used to predict properties not explicitly introduced into the learning pool. We also showed that the fast self-assembly of lipid membranes is retained by these parameters, and that the extension of their use for molecules outside the training pool, such as triglycerides, is possible.