GeTe-based alloys have been intensively considered as p-type thermoelectrics for about 50 years, yet existing literature barely discussed the thermoelectric properties of pristine GeTe at high temperatures (300–800 K). This work first backs to a fundamental understanding on the thermoelectric transport properties inherent to p-type GeTe, based on more than 50 samples synthesized with expected carrier concentrations ranging from 1 × 1020 to 3 × 1021 cm–3. A thermoelectric figure of merit zT as high as ∼1.7 is found inherent to this compound when it is optimally doped with a Hall carrier concentration of 2.2 ± 10% × 1020 cm–3, offering a reference substance to expose the origins for the high zT in historical GeTe-based alloys. Guided by the above knowledge, further alloying Te with Se in samples with an optimal carrier concentration enables a reduction on the lattice thermal conductivity by ∼40% and eventually leads to a further enhancement on zT (up to 2.0) by ∼20%. This work demonstrates not only GeTe as an inherently high performance thermoelectric matrix compound but also its availability for further improvements by additional strategies.