Jupiter’s moon Ganymede might be in possession of a subsurface ocean located between two ice layers. However, from Galileo data it is not possible to unambiguously infer the thickness and densities of the individual layers. The upcoming icy satellite mission JUICE (JUpiter ICy moons Explorer) will have the possibility to perform more detailed investigations of Ganymede’s interior structure with the radio science experiment 3GM and the GAnymede Laser Altimeter (GALA). Here we investigate the possibility to derive the rotational state of the outer ice shell by using topography measured by laser altimetry. We discuss two different methods to invert synthetic laser altimetry data. Method 1 is based on a spherical harmonics expansion and Method 2 solves for B-splines on a rectangular grid. While Method 1 has significant limitations due to the omission of high degrees of the global expansion, Method 2 leads to stable results allowing for an estimate of the in-orbit measurement accuracy. We estimate that GALA can measure the amplitude of Ganymede’s librations with an accuracy of 2.5–6.6 µrad (6.6–17.4 m at the equator). This allows for determining the thickness of an elastic ice shell, if decoupled from the deeper interior by a subsurface ocean, to about an accuracy of 24–65 km.