A comprehensive study of ZrCr2 Laves phases is important for both fundamental research and technological applications. The ZrCr2 compound is a typical precipitate observed in Zr-based alloys including the newly developed Cr-coated Zr cladding known as Accident Tolerant Fuel cladding. The brittle behavior of the Laves phases and the low melting point at the interface zone between the precipitates and the Zr matrix are considered as governing the thermomechanical behaviors of these newly developed nuclear fuel claddings for normal operating conditions but more dramatically in case of Loss Of Coolant Accident (LOCA) conditions. The aim of the present study is to investigate the various ZrCr2 Laves polymorphs and their thermodynamic features particularly where conflicts exist in the literature. Based on diffraction experiments of annealed samples, it has been established that the transformation from the C14 high-temperature form to the C15 low-temperature form is of displacive nature without the C36 polymorph forming as an intermediate phase. The stable and metastable domains of C14 and C15 and their thermodynamic properties have been determined. The specific heat of both C14 and C15 types was measured over a wide range of temperatures from 2 to 1063 K by coupling relaxation calorimetry and DSC. The experimental data were fitted using a modified Einstein model. The room temperature entropies of the C14 and C15 phases were evaluated. The enthalpy of formation was measured for the first time using drop solution calorimetry in liquid Al at 1173 K in a Tian–Calvet calorimeter. The experimental value is in good agreement with Density Functional Theory (DFT) calculations. Finally, all these new results are discussed regarding the abundant literature on the ZrCr2 Laves phases.