The stronger decrease in hydrophobic compared to hydrophilic water corroborates entropically driven de-solvation events of the hydrophobic polymer surface with increasing thionation (and decreasing LCST values); this effect seems more pronounced than the described decrease in hydrogen bonding and, similar to the measured Tcp values, shows a linear trend. While our simulations involved much smaller polymer chains than the experimentally investigated structures, we expect the observed changes to be even more notable at increased chain lengths where entropic effects become more influential.