The molar heat capacities of the Fe2Nb and Fe7Nb6 intermetallic compounds are reported here for the first time. The results were obtained via Differential Scanning Calorimetry (DSC) measurements, performed in a temperature range between 348 and 1038 K. The alloys were prepared by arc-melting high purity metals under argon flux and later heat-treated at 1200 ∘C for 336 h encapsulated in quartz tubes under argon to ensure thermodynamic equilibrium. The resulting samples were then characterized using X-Ray Diffractometry (XRD) and Scanning Electron Microscopy (SEM). The heat-capacity DSC measurements were carried out using an alternating step method with 20 and 50 K steps, with the resulting Cp associated with the midpoint of each temperature interval. A fit to a simplified Cp(T) curve was employed, due to the scatter in the data. Quasi-Harmonic Approximation (QHA) calculations were also performed, showing a good agreement with the measured values. Experimental results of heat capacity, along with other thermodynamic properties and phase equilibria, are key information for binary and ternary systems, specially for CALPHAD-type assessments. The results were therefore compared with the Kopp-Neumann approximation, used in recent assessments, showing that the parameters of both compounds can be improved in current CALPHAD databases, which motivates future work on the Fe-Nb system.