Andradite, ideal end-member formula Ca 3 Fe 3þ 2 Si 3 O 12 , is one of the common rock-forming garnets found in the Earth's crust. There are several outstanding questions regarding andradite's thermodynamic and physical property behavior. Three issues are: i) Could there be differences in the thermodynamic properties, namely heat capacity, C p , between synthetic and natural andradite crystals, as observed in the Ca-garnet grossular, Ca 3 Al 2 Si 3 O 12 ? ii) What is the thermal nature of the low-temperature magnetic-phasetransition behavior of andradite? and iii) How quantitative are older published calorimetric (i.e., adiabatic and DSC) heat-capacity results? In this work, four natural nearly end-member single crystals and two synthetic polycrystalline andradite samples were carefully characterized by optical microscope examination, X-ray powder diffraction, microprobe analysis, and IR and UV/VIS single-crystal spectroscopy. The IR spectra of the different samples commonly show a main intense OH À stretching band located at 3563 cm À1 , but other OH À bands can sometimes be observed as well. Structural OH À concentrations, calculated from the IR spectra, vary from about 0.006 to 0.240 wt% H 2 O. The UV/VIS spectra indicate that there can be slight, but not fully understood, differences in the electronic state between synthetic and natural andradite crystals. The C p behavior was determined by relaxation calorimetry between 2 and 300 K and by differential scanning calorimetry (DSC) methods between 150/300 and 700/950 K, employing the same andradite samples that were used for the other characterization measurements. The low-temperature C p results show a magnetic phase transition with a Néel temperature of 11.3 ± 0.2 K, which could be slightly affected by the precise electronic state of Fe 2þ/3þ in the crystals. The published adiabatic calorimetry results on andradite do not provide a full and correct thermal description of this magnetic transition. The calorimetric C p measurements give a best estimate for the standard third-law entropy at 298.15 K for andradite of S o ≈ 324 ± 2 J/mol · K vs. the value of 316.4 ± 2.0 J/mol · K, as given in an early adiabatic investigation. Both natural and synthetic crystals give similar S o values within experimental uncertainty of about 1.0%, but one natural andradite, richer in OH, may have a very slightly higher value around S o ≈ 326 J/mol · K. Low-temperature DSC measurements made below 298 K agree excellently with those from relaxation calorimetry. The DSC measurements above 298 K show a similarity in C p behavior among natural and synthetic andradites. A C p polynomial for use above room temperature to approximately 1000 K was calculated from the data on synthetic andradite giving: C p (J/mol · K) = 599.09 (±14) À 2709.5 (±480) · T À0.5 À 1.3866 (±0.26) · 10 7 · T À2 þ 1.6052 (±0.42) · 10 9 · T À3 .