Based on previous applications of laser altimetry to planetary geodesy at GSFC, we use the recently developed PyXover software package to analyze altimetric crossovers from the Mercury Laser Altimeter (MLA). Using PyXover, we place new constraints on Mercury’s geodetic parameters via least‐squares minimization of crossover discrepancies. We simultaneously solve for orbital corrections for each MLA ground track, for the geodetic parameters of the IAU‐recommended orientation model for Mercury (pole right‐ascension and declination coordinates, prime meridian rotation rate and librations), and for the Mercury’s Love number h2. We calibrate the formal errors of our solution based on closed‐loop simulations and on the level of robustness against a priori values, data selection, and parametrization. Our solution of the Mercury’s rotational parameters is consistent with published values. In particular, our new estimate for the orientation of the pole places Mercury in a Cassini state, with an obliquity ϵ = 2.031 ± 0.03 arcmin compatible with previous “surface” related measurements. Moreover, we provide a first data‐based estimate of the Love number h2 = 1.55 ± 0.65. The latter is consistent with expectations from models of Mercury’s interior, although its precision does not enable their refinement.